Plasmonic nanoantennas provide unique opportunities for precise control of light–matter coupling in surface-enhanced infrared absorption(SEIRA)spectroscopy,but most of the resonant systems realized so far suffer from...Plasmonic nanoantennas provide unique opportunities for precise control of light–matter coupling in surface-enhanced infrared absorption(SEIRA)spectroscopy,but most of the resonant systems realized so far suffer from the obstacles of low sensitivity,narrow bandwidth,and asymmetric Fano resonance perturbations.Here,we demonstrated an overcoupled resonator with a high plasmon-molecule coupling coefficient(μ)(OC-Hμresonator)by precisely controlling the radiation loss channel,the resonator-oscillator coupling channel,and the frequency detuning channel.We observed a strong dependence of the sensing performance on the coupling state,and demonstrated that OC-Hμresonator has excellent sensing properties of ultra-sensitive(7.25%nm^(−1)),ultra-broadband(3–10μm),and immune asymmetric Fano lineshapes.These characteristics represent a breakthrough in SEIRA technology and lay the foundation for specific recognition of biomolecules,trace detection,and protein secondary structure analysis using a single array(array size is 100×100μm^(2)).In addition,with the assistance of machine learning,mixture classification,concentration prediction and spectral reconstruction were achieved with the highest accuracy of 100%.Finally,we demonstrated the potential of OC-Hμresonator for SARS-CoV-2 detection.These findings will promote the wider application of SEIRA technology,while providing new ideas for other enhanced spectroscopy technologies,quantum photonics and studying light–matter interactions.展开更多
Water electrolysis poses a significant challenge for balancing catalytic activity and stability of oxygen evolution reaction(OER)electrocatalysts.In this study,we address this challenge by constructing asymmetric redo...Water electrolysis poses a significant challenge for balancing catalytic activity and stability of oxygen evolution reaction(OER)electrocatalysts.In this study,we address this challenge by constructing asymmetric redox chemistry through elaborate surface OO–Ru–OH and bulk Ru–O–Ni/Fe coordination moieties within single-atom Ru-decorated defective NiFe LDH nanosheets(Ru@d-NiFe LDH)in conjunction with strong metal-support interactions(SMSI).Rigorous spectroscopic characterization and theoretical calculations indicate that single-atom Ru can delocalize the O 2p electrons on the surface and optimize d-electron configurations of metal atoms in bulk through SMSI.The^(18)O isotope labeling experiment based on operando differential electrochemical mass spectrometry(DEMS),chemical probe experiments,and theoretical calculations confirm the encouraged surface lattice oxygen,stabilized bulk lattice oxygen,and enhanced adsorption of oxygen-containing intermediates for bulk metals in Ru@d-NiFe LDH,leading to asymmetric redox chemistry for OER.The Ru@d-NiFe LDH electrocatalyst exhibits exceptional performance with an overpotential of 230 mV to achieve 10 mA cm^(−2)and maintains high robustness under industrial current density.This approach for achieving asymmetric redox chemistry through SMSI presents a new avenue for developing high-performance electrocatalysts and instills confidence in its industrial applicability.展开更多
Tree interactions are essential for the structure,dynamics,and function of forest ecosystems,but variations in the architecture of life-stage interaction networks(LSINs)across forests is unclear.Here,we constructed 16...Tree interactions are essential for the structure,dynamics,and function of forest ecosystems,but variations in the architecture of life-stage interaction networks(LSINs)across forests is unclear.Here,we constructed 16 LSINs in the mountainous forests of northwest Hebei,China based on crown overlap from four mixed forests with two dominant tree species.Our results show that LSINs decrease the complexity of stand densities and basal areas due to the interaction cluster differentiation.In addition,we found that mature trees and saplings play different roles,the first acting as“hub”life stages with high connectivity and the second,as“bridges”controlling information flow with high centrality.Across the forests,life stages with higher importance showed better parameter stability within LSINs.These results reveal that the structure of tree interactions among life stages is highly related to stand variables.Our efforts contribute to the understanding of LSIN complexity and provide a basis for further research on tree interactions in complex forest communities.展开更多
In the current information society, the dissemination mechanisms and evolution laws of individual or collective opinions and their behaviors are the research hot topics in the field of opinion dynamics. First, in this...In the current information society, the dissemination mechanisms and evolution laws of individual or collective opinions and their behaviors are the research hot topics in the field of opinion dynamics. First, in this paper, a two-layer network consisting of an individual-opinion layer and a collective-opinion layer is constructed, and a dissemination model of opinions incorporating higher-order interactions(i.e. OIHOI dissemination model) is proposed. Furthermore, the dynamic equations of opinion dissemination for both individuals and groups are presented. Using Lyapunov's first method,two equilibrium points, including the negative consensus point and positive consensus point, and the dynamic equations obtained for opinion dissemination, are analyzed theoretically. In addition, for individual opinions and collective opinions,some conditions for reaching negative consensus and positive consensus as well as the theoretical expression for the dissemination threshold are put forward. Numerical simulations are carried to verify the feasibility and effectiveness of the proposed theoretical results, as well as the influence of the intra-structure, inter-connections, and higher-order interactions on the dissemination and evolution of individual opinions. The main results are as follows.(i) When the intra-structure of the collective-opinion layer meets certain characteristics, then a negative or positive consensus is easier to reach for individuals.(ii) Both negative consensus and positive consensus perform best in mixed type of inter-connections in the two-layer network.(iii) Higher-order interactions can quickly eliminate differences in individual opinions, thereby enabling individuals to reach consensus faster.展开更多
Ultrafast transmission electron microscope(UTEM) with the multimodality of time-resolved diffraction, imaging,and spectroscopy provides a unique platform to reveal the fundamental features associated with the interact...Ultrafast transmission electron microscope(UTEM) with the multimodality of time-resolved diffraction, imaging,and spectroscopy provides a unique platform to reveal the fundamental features associated with the interaction between free electrons and matter. In this review, we summarize the principles, instrumentation, and recent developments of the UTEM and its applications in capturing dynamic processes and non-equilibrium transient states. The combination of the transmission electron microscope with a femtosecond laser via the pump–probe method guarantees the high spatiotemporal resolution, allowing the investigation of the transient process in real, reciprocal and energy spaces. Ultrafast structural dynamics can be studied by diffraction and imaging methods, revealing the coherent acoustic phonon generation and photoinduced phase transition process. In the energy dimension, time-resolved electron energy-loss spectroscopy enables the examination of the intrinsic electronic dynamics of materials, while the photon-induced near-field electron microscopy extends the application of the UTEM to the imaging of optical near fields with high real-space resolution. It is noted that light–free-electron interactions have the ability to shape electron wave packets in both longitudinal and transverse directions, showing the potential application in the generation of attosecond electron pulses and vortex electron beams.展开更多
Individual superatoms are assembled into more complicated nanostructures to diversify their physical properties.Magnetism of assembled superatoms remains,however,ambiguous,particularly in terms of its distance depende...Individual superatoms are assembled into more complicated nanostructures to diversify their physical properties.Magnetism of assembled superatoms remains,however,ambiguous,particularly in terms of its distance dependence.Here,we report density functional theory calculations on the distance-dependent magnetism of transition metal embedded Au_(6)Te_(8)Se_(12)(ATS)superatomic dimers.Among the four considered transition metals,which include V,Cr,Mn and Fe,the Cr-embedded Au_(6)Te_(12)Se_(8)(Cr@ATS)is identified as the most suitable for exploring the inter-superatomic distancedependent magnetism.We thus focused on Cr@ATS superatomic dimers and found an inter-superatomic magnetizationdistance oscillation where three transitions occur for magnetic ordering and/or anisotropy at different inter-superatomic distances.As the inter-superatomic distance elongates,a ferromagnetism(FM)-to-antiferromagnetic(AFM)transition and a sequential AFM-to-FM transition occur,ascribed to competitions among Pauli repulsion and kinetic-energy-gains in formed inter-superatomic Cr-Au-Au-Cr covalent bonds and Te-Te quasi-covalent bonds.For the third transition,in-plane electronic hybridization contributes to the stabilization of the AFM configuration.This work unveils two mechanisms for tuning magnetism through non-covalent interactions and provides a strategy for manipulating magnetism in superatomic assemblies.展开更多
Light–matter interactions in two-dimensional(2D)materials have been the focus of research since the discovery of graphene.The light–matter interaction length in 2D materials is,however,much shorter than that in bulk...Light–matter interactions in two-dimensional(2D)materials have been the focus of research since the discovery of graphene.The light–matter interaction length in 2D materials is,however,much shorter than that in bulk materials owing to the atomic nature of 2D materials.Plasmonic nanostructures are usually integrated with 2D materials to enhance the light–matter interactions,offering great opportunities for both fundamental research and technological applications.Nanoparticle-on-mirror(NPo M)structures with extremely confined optical fields are highly desired in this aspect.In addition,2D materials provide a good platform for the study of plasmonic fields with subnanometer resolution and quantum plasmonics down to the characteristic length scale of a single atom.A focused and up-to-date review article is highly desired for a timely summary of the progress in this rapidly growing field and to encourage more research efforts in this direction.In this review,we will first introduce the basic concepts of plasmonic modes in NPo M structures.Interactions between plasmons and quasi-particles in 2D materials,e.g.,excitons and phonons,from weak to strong coupling and potential applications will then be described in detail.Related phenomena in subnanometer metallic gaps separated by 2D materials,such as quantum tunneling,will also be touched.We will finally discuss phenomena and physical processes that have not been understood clearly and provide an outlook for future research.We believe that the hybrid systems of2D materials and NPo M structures will be a promising research field in the future.展开更多
Recently,lipid nanoparticles(LNPs)have been extensively investigated as non-viral carriers of nucleic acid vaccines due to their high transport efficiency,safety,and straightforward production and scalability.However,...Recently,lipid nanoparticles(LNPs)have been extensively investigated as non-viral carriers of nucleic acid vaccines due to their high transport efficiency,safety,and straightforward production and scalability.However,the molecular mechanism underlying the interactions between nucleic acids and phospholipid bilayers within LNPs remains elusive.In this study,we employed the all-atom molecular dynamics simulation to investigate the interactions between single-stranded nucleic acids and a phospholipid bilayer.Our findings revealed that hydrophilic bases,specifically G in single-stranded RNA(ssRNA)and single-stranded DNA(ssDNA),displayed a higher propensity to form hydrogen bonds with phospholipid head groups.Notably,ssRNA exhibited stronger binding energy than ssDNA.Furthermore,divalent ions,particularly Ca2+,facilitated the binding of ssRNA to phospholipids due to their higher binding energy and lower dissociation rate from phospholipids.Overall,our study provides valuable insights into the molecular mechanisms underlying nucleic acidphospholipid interactions,with potential implications for the nucleic acids in biotherapies,particularly in the context of lipid carriers.展开更多
In this paper, we study the flocking behavior of a thermodynamic Cucker–Smale model with local velocity interactions. Using the spectral gap of a connected stochastic matrix, together with an elaborate estimate on pe...In this paper, we study the flocking behavior of a thermodynamic Cucker–Smale model with local velocity interactions. Using the spectral gap of a connected stochastic matrix, together with an elaborate estimate on perturbations of a linearized system, we provide a sufficient framework in terms of initial data and model parameters to guarantee flocking. Moreover, it is shown that the system achieves a consensus at an exponential rate.展开更多
This review provides a comprehensive overview of the progress in light-material interactions(LMIs),focusing on lasers and flash lights for energy conversion and storage applications.We discuss intricate LMI parameters...This review provides a comprehensive overview of the progress in light-material interactions(LMIs),focusing on lasers and flash lights for energy conversion and storage applications.We discuss intricate LMI parameters such as light sources,interaction time,and fluence to elucidate their importance in material processing.In addition,this study covers various light-induced photothermal and photochemical processes ranging from melting,crystallization,and ablation to doping and synthesis,which are essential for developing energy materials and devices.Finally,we present extensive energy conversion and storage applications demonstrated by LMI technologies,including energy harvesters,sensors,capacitors,and batteries.Despite the several challenges associated with LMIs,such as complex mechanisms,and high-degrees of freedom,we believe that substantial contributions and potential for the commercialization of future energy systems can be achieved by advancing optical technologies through comprehensive academic research and multidisciplinary collaborations.展开更多
The modulation of metal-support interfacial interaction is significant but challenging in the design of high-efficiency and high-stability supported catalysts.Here,we report a synthetic strategy to upgrade Cu-CeO_(2)i...The modulation of metal-support interfacial interaction is significant but challenging in the design of high-efficiency and high-stability supported catalysts.Here,we report a synthetic strategy to upgrade Cu-CeO_(2)interfacial interaction by the pyrolysis of mixed metal-organic framework(MOF)structure.The obtained highly dispersed Cu/CeO_(2)-MOF catalyst via this strategy was used to catalyze water-gas shift reaction(WGSR),which exhibited high activity of 40.5μmolCOgcat^(-1).s^(-1)at 300℃and high stability of about 120 h.Based on comprehensive studies of electronic structure,pyrolysis strategy has significant effect on enhancing metal-support interaction and then stabilizing interfacial Cu^(+)species under reaction conditions.Abundant Cu^(+)species and generated oxygen vacancies over Cu/CeO_(2)-MOF catalyst played a key role in CO molecule activation and H2O molecule dissociation,respectively.Both collaborated closely and then promoted WGSR catalytic performance in comparison with traditio nal supported catalysts.This study shall offer a robust approach to harvest highly dispersed catalysts with finely-tuned metal-support interactions for stabilizing the most interfacial active metal species in diverse heterogeneous catalytic reactions.展开更多
Studies showed that complexation of polyphenols with milk allergens reduced their immunogenic potential.However,the relationship between structures of polyphenols and their hypoallergenic effects on milk allergens in ...Studies showed that complexation of polyphenols with milk allergens reduced their immunogenic potential.However,the relationship between structures of polyphenols and their hypoallergenic effects on milk allergens in association with physiological and conformational changes of the complexes remain unclear.In this study,polyphenols from eight botanical sources were extracted to prepare non-covalent complexes withβ-lactoglobulin(β-LG),a major allergen in milk.The dominant phenolic compounds bound toβ-LG with a diminished allergenicity were identified to investigate their respective role on the structural and allergenic properties ofβ-LG.Extracts from Vaccinium fruits and black soybeans were found to have great inhibitory effects on the IgE-and IgG-binding abilities ofβ-LG.Among the fourteen structure-related phenolic compounds,flavonoids and tannins with larger MWs and multi-hydroxyl substituents,notably rutin,EGCG,and ellagitannins were more potent to elicit changes on the conformational structures ofβ-LG to decrease the allergenicity of complexedβ-LG.Correlation analysis further demonstrated that a destabilized secondary structure and protein depolymerization caused by polyphenol-binding were closely related to the allergenicity property of formed complexes.This study provides insights into the understanding of structure-allergenicity relationship ofβ-LG-polyphenol interactions and would benefit the development of polyphenol-fortified matrices with hypoallergenic potential.展开更多
Spin-orbit optical phenomena pertain to the wider class of electromagnetic effects originating from the interaction of the photon spin with the spatial structure and propagation characteristics of an optical wave,medi...Spin-orbit optical phenomena pertain to the wider class of electromagnetic effects originating from the interaction of the photon spin with the spatial structure and propagation characteristics of an optical wave,mediated by suitable optical media.There are many emerging photonic applications of spin-orbit interactions(SOI)of light,such as control of the optical wave propagation via the spin,enhanced optical manipulation,and generation of structured optical fields.Unfortunately,current applications are based on symmetric SOI,that is,the behaviours of polarized photons with two opposite spins are opposite,leading to the limit of spin-based multiplexers.The symmetry of SOI can be broken in our proposed metasurfaces,consisting of spatially varying birefringence,which can arbitrarily and independently build SOI for two opposite spins without reduction of optical energy usage.We obtain three kinds of dual-functional metasurfaces at visible and infrared wavelengths with high efficiency.Our concept of generation of asymmetric SOI for two spins,using anisotropic metasurfaces,will open new degrees of freedoms for building new types of spin-controlled multifunctional shared-aperture devices for the generation of complex structured optical fields.展开更多
Realizing the uniform dispersion of nanocarbons such as carbon nanotube and graphene in metals, is an essential prerequisite to fully exhibit their enhancement effect in mechanical, thermal, and electrical properties ...Realizing the uniform dispersion of nanocarbons such as carbon nanotube and graphene in metals, is an essential prerequisite to fully exhibit their enhancement effect in mechanical, thermal, and electrical properties of metal matrix composites(MMCs). In this work, we propose an effective method to achieve uniform distribution of nanocarbons in various metal flakes through a slurry-based method. It relies on the electrostatic interactions between the negatively charged nanocarbons and the positively charged metal flakes when mixed in slurry. For case study, flake metal powders(Al, Mg, Ti,Fe, and Cu) were positively charged in aqueous suspension by spontaneous ionization or cationic surface modification. While nanocarbons, given examples as carboxylic multi-walled carbon nanotubes, pristine single-walled carbon nanotube, and carbon nanotube–graphene oxide hybrid were negatively charged by the ionization of oxygen-containing functional groups or anionic surfactant. It was found that through the electrostatic interaction mechanism, all kinds of nanocarbons can be spontaneously and efficiently adsorbed onto the surface of various metal flakes. The development of such a versatile method would provide us great opportunities to fabricate advanced MMCs with appealing properties.展开更多
Using the split-step Fourier transform method, we numerically investigate the generation of breathing solitons in the propagation and interactions of Airy–Gaussian（AiG） beams in a cubic–quintic nonlinear medium in...Using the split-step Fourier transform method, we numerically investigate the generation of breathing solitons in the propagation and interactions of Airy–Gaussian（AiG） beams in a cubic–quintic nonlinear medium in one transverse dimension. We show that the propagation of single AiG beams can generate stable breathing solitons that do not accelerate within a certain initial power range. The propagation direction of these breathing solitons can be controlled by introducing a launch angle to the incident AiG beams. When two AiG beams accelerated in opposite directions interact with each other,different breathing solitons and soliton pairs are observed by adjusting the phase shift, the beam interval, the amplitudes,and the light field distribution of the initial AiG beams.展开更多
The reason for the asymmetry phenomenon of shock/boundary layer interactions(SBLI)in a completely symmetric nozzle with symmetric flow conditions is still an open question.A model for the asymmetry of nozzle flows was...The reason for the asymmetry phenomenon of shock/boundary layer interactions(SBLI)in a completely symmetric nozzle with symmetric flow conditions is still an open question.A model for the asymmetry of nozzle flows was proposed based on the properties of fluid entrainment in the mixing layer and momentum conservation.The asymmetry model is deduced based on the nozzle flow with restricted shock separation,and is still applicable for free shock separation.Flow deflection angle at nozzle exit is deduced from this model.Steady numerical simulations are conducted to model the asymmetry of the SBLIs in a planar convergent-divergent nozzle tested by previous researchers.The obtained values of deflection angle based on the numerical results of forced symmetric nozzle flows can judge the asymmetry of flows in a nozzle at some operations.It shows that the entrainment of shear layer on the separation induced by SBLTs is one of the reasons for the asymmetry in the confined SBLIs.展开更多
Research on the spatial patterns of tree populations is critical for understanding the structure and dynamic processes of forests.However,little is known about how the underlying drivers shape these patterns and speci...Research on the spatial patterns of tree populations is critical for understanding the structure and dynamic processes of forests.However,little is known about how the underlying drivers shape these patterns and species interactions in forest systems.In this study,spatial point pattern analysis investigated the combined eff ects of intraspecifi c interactions and environmental heterogeneity on the spatial structure and internal maintenance mechanisms of Picea crassifolia in the Qilian Mountain National Nature Reserve,China.Data were obtained from a 10.2-ha dynamic monitoring plot(DMP)and sixteen 0.04-ha elevation gradient plots(EGPs).Under complete spatial randomness,both mature trees and saplings in the DMP demonstratedlarge-scale aggregation with negative correlations.In EGPs,saplings were clustered in small mesoscales,mature trees were randomly distributed,and the interactions of saplingstrees at all elevations were not correlated.By eliminating the interference of environmental heterogeneity through the inhomogeneous Poisson process,saplings in the DMP and EGPs were clustered in small scales and trees randomly distributed.Intraspecifi c associations were negatively correlated,in the DMP and at low elevations,and no correlations in high elevations of EGPs.In the vertical scale,saplings showed a small-scale aggregation pattern with increase in elevation,and the aggregation degree fi rst decreased and then increased.The interactions of saplings-trees and saplings–saplings showed inhibitions at small scales,with the degree of inhibition gradually decreasing.Spatial patterns and associations of adults–adults did not change signifi-cantly.The results revealed that intraspecifi c interactions and environmental heterogeneity regulated the spatial patterns of P.crassifolia at small and large scales,respectively.Environmental heterogeneity might be the most decisive factor aff ecting the spatial patterns of saplings,while trees were more aff ected by intraspecifi c interactions.Moreover,competition between trees in this area could be more common than facilitation for the growth and development of individuals.展开更多
The depletion interactions between two large-spheres immersed in a fluid of small spheres under unsymmetrical geometrical confinement are studied through the acceptance ratio method. The numerical results show that no...The depletion interactions between two large-spheres immersed in a fluid of small spheres under unsymmetrical geometrical confinement are studied through the acceptance ratio method. The numerical results show that no matter whether the volume fraction is large or small, both the depletion potential and depletion force are affected by the presence of the two plates; the closer the two large spheres are to the plate, the larger the effects of the unsymmetrical confinements.展开更多
Hydrogen is one of the most attractive renewables for future energy application,therefore it is vital to develop cost-effective and highlyefficient electrocatalysts for the hydrogen evolution reaction(HER)to promote t...Hydrogen is one of the most attractive renewables for future energy application,therefore it is vital to develop cost-effective and highlyefficient electrocatalysts for the hydrogen evolution reaction(HER)to promote the generation of hydrogen from mild methods.In this work,Co–Mo phosphide nanosheets with the adjustable ratio of Co and Mo were fabricated on carbon cloth by a facile hydrothermal-annealing method.Owing to the unique nanostructures,abundant active surfaces and small resistance were achieved.Excellent electrocatalytic performances are obtained,such as the small overpotential of^67.3 mV to realize a current density of 10 mA cm^(-2) and a Tafel slope of 69.9 mV dec^(-1).Rapid recovery of the current response under multistep chronoamperometry is realized and excellent stability retained after the CV test for 2000 cycles.The change of electronic states of different elements was carefully studied which suggested the optimal electrochemical performance can be realized by tuning phosphorous and metal interactions.展开更多
Starting from the extended tanh-function method （ETM） based on the mapping method, the variable separation solutions of the （2＋1）-dimensional asymmetric Nizhnik Novikov Veselov （ANNV） system are derived. By fur...Starting from the extended tanh-function method （ETM） based on the mapping method, the variable separation solutions of the （2＋1）-dimensional asymmetric Nizhnik Novikov Veselov （ANNV） system are derived. By further study, we find that these variable separation solutions are seemingly independent of but actually dependent on each other. Based on the variable separation solution and by choosing appropriate functions, some novel and interesting interactions between special solitons, such as bell-like compacton, peakon-like compacton and compacton-like semifoldon, are investigated.展开更多
基金supported by A*STAR under the“Nanosystems at the Edge”program(Grant No.A18A4b0055)Ministry of Education(MOE)under the research grant of R-263-000-F18-112/A-0009520-01-00+1 种基金National Research Foundation Singapore grant CRP28-2022-0038the Reimagine Re-search Scheme(RRSC)Project(Grant A-0009037-02-00&A0009037-03-00)at National University of Singapore.
文摘Plasmonic nanoantennas provide unique opportunities for precise control of light–matter coupling in surface-enhanced infrared absorption(SEIRA)spectroscopy,but most of the resonant systems realized so far suffer from the obstacles of low sensitivity,narrow bandwidth,and asymmetric Fano resonance perturbations.Here,we demonstrated an overcoupled resonator with a high plasmon-molecule coupling coefficient(μ)(OC-Hμresonator)by precisely controlling the radiation loss channel,the resonator-oscillator coupling channel,and the frequency detuning channel.We observed a strong dependence of the sensing performance on the coupling state,and demonstrated that OC-Hμresonator has excellent sensing properties of ultra-sensitive(7.25%nm^(−1)),ultra-broadband(3–10μm),and immune asymmetric Fano lineshapes.These characteristics represent a breakthrough in SEIRA technology and lay the foundation for specific recognition of biomolecules,trace detection,and protein secondary structure analysis using a single array(array size is 100×100μm^(2)).In addition,with the assistance of machine learning,mixture classification,concentration prediction and spectral reconstruction were achieved with the highest accuracy of 100%.Finally,we demonstrated the potential of OC-Hμresonator for SARS-CoV-2 detection.These findings will promote the wider application of SEIRA technology,while providing new ideas for other enhanced spectroscopy technologies,quantum photonics and studying light–matter interactions.
基金supported by the Guangdong Basic and Applied Basic Research Foundation(2021B1515120072)the Natural Science Foundation of China(22279096 and T2241003)the Fundamental Research Funds for the Central Universities(WUT:2023IVA094).
文摘Water electrolysis poses a significant challenge for balancing catalytic activity and stability of oxygen evolution reaction(OER)electrocatalysts.In this study,we address this challenge by constructing asymmetric redox chemistry through elaborate surface OO–Ru–OH and bulk Ru–O–Ni/Fe coordination moieties within single-atom Ru-decorated defective NiFe LDH nanosheets(Ru@d-NiFe LDH)in conjunction with strong metal-support interactions(SMSI).Rigorous spectroscopic characterization and theoretical calculations indicate that single-atom Ru can delocalize the O 2p electrons on the surface and optimize d-electron configurations of metal atoms in bulk through SMSI.The^(18)O isotope labeling experiment based on operando differential electrochemical mass spectrometry(DEMS),chemical probe experiments,and theoretical calculations confirm the encouraged surface lattice oxygen,stabilized bulk lattice oxygen,and enhanced adsorption of oxygen-containing intermediates for bulk metals in Ru@d-NiFe LDH,leading to asymmetric redox chemistry for OER.The Ru@d-NiFe LDH electrocatalyst exhibits exceptional performance with an overpotential of 230 mV to achieve 10 mA cm^(−2)and maintains high robustness under industrial current density.This approach for achieving asymmetric redox chemistry through SMSI presents a new avenue for developing high-performance electrocatalysts and instills confidence in its industrial applicability.
基金This study was supported by the National Water Pollution Control and Treatment Science and Technology Major Project(2017ZX07101-002).
文摘Tree interactions are essential for the structure,dynamics,and function of forest ecosystems,but variations in the architecture of life-stage interaction networks(LSINs)across forests is unclear.Here,we constructed 16 LSINs in the mountainous forests of northwest Hebei,China based on crown overlap from four mixed forests with two dominant tree species.Our results show that LSINs decrease the complexity of stand densities and basal areas due to the interaction cluster differentiation.In addition,we found that mature trees and saplings play different roles,the first acting as“hub”life stages with high connectivity and the second,as“bridges”controlling information flow with high centrality.Across the forests,life stages with higher importance showed better parameter stability within LSINs.These results reveal that the structure of tree interactions among life stages is highly related to stand variables.Our efforts contribute to the understanding of LSIN complexity and provide a basis for further research on tree interactions in complex forest communities.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.72031009 and 61473338)。
文摘In the current information society, the dissemination mechanisms and evolution laws of individual or collective opinions and their behaviors are the research hot topics in the field of opinion dynamics. First, in this paper, a two-layer network consisting of an individual-opinion layer and a collective-opinion layer is constructed, and a dissemination model of opinions incorporating higher-order interactions(i.e. OIHOI dissemination model) is proposed. Furthermore, the dynamic equations of opinion dissemination for both individuals and groups are presented. Using Lyapunov's first method,two equilibrium points, including the negative consensus point and positive consensus point, and the dynamic equations obtained for opinion dissemination, are analyzed theoretically. In addition, for individual opinions and collective opinions,some conditions for reaching negative consensus and positive consensus as well as the theoretical expression for the dissemination threshold are put forward. Numerical simulations are carried to verify the feasibility and effectiveness of the proposed theoretical results, as well as the influence of the intra-structure, inter-connections, and higher-order interactions on the dissemination and evolution of individual opinions. The main results are as follows.(i) When the intra-structure of the collective-opinion layer meets certain characteristics, then a negative or positive consensus is easier to reach for individuals.(ii) Both negative consensus and positive consensus perform best in mixed type of inter-connections in the two-layer network.(iii) Higher-order interactions can quickly eliminate differences in individual opinions, thereby enabling individuals to reach consensus faster.
基金supported by the National Natural Science Foundation of China (Grant Nos.U22A6005 and 12074408)the National Key Research and Development Program of China (Grant No.2021YFA1301502)+7 种基金Guangdong Major Scientific Research Project (Grant No.2018KZDXM061)Youth Innovation Promotion Association of CAS (Grant No.2021009)Scientific Instrument Developing Project of the Chinese Academy of Sciences (Grant Nos.YJKYYQ20200055,ZDKYYQ2017000,and 22017BA10)Strategic Priority Research Program (B) of the Chinese Academy of Sciences (Grant Nos.XDB25000000 and XDB33010100)Beijing Municipal Science and Technology Major Project (Grant No.Z201100001820006)IOP Hundred Talents Program (Grant No.Y9K5051)Postdoctoral Support Program of China (Grant No.2020M670501)the Synergetic Extreme Condition User Facility (SECUF)。
文摘Ultrafast transmission electron microscope(UTEM) with the multimodality of time-resolved diffraction, imaging,and spectroscopy provides a unique platform to reveal the fundamental features associated with the interaction between free electrons and matter. In this review, we summarize the principles, instrumentation, and recent developments of the UTEM and its applications in capturing dynamic processes and non-equilibrium transient states. The combination of the transmission electron microscope with a femtosecond laser via the pump–probe method guarantees the high spatiotemporal resolution, allowing the investigation of the transient process in real, reciprocal and energy spaces. Ultrafast structural dynamics can be studied by diffraction and imaging methods, revealing the coherent acoustic phonon generation and photoinduced phase transition process. In the energy dimension, time-resolved electron energy-loss spectroscopy enables the examination of the intrinsic electronic dynamics of materials, while the photon-induced near-field electron microscopy extends the application of the UTEM to the imaging of optical near fields with high real-space resolution. It is noted that light–free-electron interactions have the ability to shape electron wave packets in both longitudinal and transverse directions, showing the potential application in the generation of attosecond electron pulses and vortex electron beams.
基金financial support from the National Key R&D Program of China(Grant No.2023YFA1406500)the National Natural Science Foundation of China(Grant Nos.11974422,12104504,and 12204534)+1 种基金the Fundamental Research Funds for the Central Universitiesthe Research Funds of Renmin University of China(Grant No.22XNKJ30)。
文摘Individual superatoms are assembled into more complicated nanostructures to diversify their physical properties.Magnetism of assembled superatoms remains,however,ambiguous,particularly in terms of its distance dependence.Here,we report density functional theory calculations on the distance-dependent magnetism of transition metal embedded Au_(6)Te_(8)Se_(12)(ATS)superatomic dimers.Among the four considered transition metals,which include V,Cr,Mn and Fe,the Cr-embedded Au_(6)Te_(12)Se_(8)(Cr@ATS)is identified as the most suitable for exploring the inter-superatomic distancedependent magnetism.We thus focused on Cr@ATS superatomic dimers and found an inter-superatomic magnetizationdistance oscillation where three transitions occur for magnetic ordering and/or anisotropy at different inter-superatomic distances.As the inter-superatomic distance elongates,a ferromagnetism(FM)-to-antiferromagnetic(AFM)transition and a sequential AFM-to-FM transition occur,ascribed to competitions among Pauli repulsion and kinetic-energy-gains in formed inter-superatomic Cr-Au-Au-Cr covalent bonds and Te-Te quasi-covalent bonds.For the third transition,in-plane electronic hybridization contributes to the stabilization of the AFM configuration.This work unveils two mechanisms for tuning magnetism through non-covalent interactions and provides a strategy for manipulating magnetism in superatomic assemblies.
基金supported by the National Natural Science Foundation of China(62205183)the Research Grants Council of Hong Kong(ANR/RGC,Ref.No.A-CUHK404/21).
文摘Light–matter interactions in two-dimensional(2D)materials have been the focus of research since the discovery of graphene.The light–matter interaction length in 2D materials is,however,much shorter than that in bulk materials owing to the atomic nature of 2D materials.Plasmonic nanostructures are usually integrated with 2D materials to enhance the light–matter interactions,offering great opportunities for both fundamental research and technological applications.Nanoparticle-on-mirror(NPo M)structures with extremely confined optical fields are highly desired in this aspect.In addition,2D materials provide a good platform for the study of plasmonic fields with subnanometer resolution and quantum plasmonics down to the characteristic length scale of a single atom.A focused and up-to-date review article is highly desired for a timely summary of the progress in this rapidly growing field and to encourage more research efforts in this direction.In this review,we will first introduce the basic concepts of plasmonic modes in NPo M structures.Interactions between plasmons and quasi-particles in 2D materials,e.g.,excitons and phonons,from weak to strong coupling and potential applications will then be described in detail.Related phenomena in subnanometer metallic gaps separated by 2D materials,such as quantum tunneling,will also be touched.We will finally discuss phenomena and physical processes that have not been understood clearly and provide an outlook for future research.We believe that the hybrid systems of2D materials and NPo M structures will be a promising research field in the future.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.12222506,12347102,and 12174184).
文摘Recently,lipid nanoparticles(LNPs)have been extensively investigated as non-viral carriers of nucleic acid vaccines due to their high transport efficiency,safety,and straightforward production and scalability.However,the molecular mechanism underlying the interactions between nucleic acids and phospholipid bilayers within LNPs remains elusive.In this study,we employed the all-atom molecular dynamics simulation to investigate the interactions between single-stranded nucleic acids and a phospholipid bilayer.Our findings revealed that hydrophilic bases,specifically G in single-stranded RNA(ssRNA)and single-stranded DNA(ssDNA),displayed a higher propensity to form hydrogen bonds with phospholipid head groups.Notably,ssRNA exhibited stronger binding energy than ssDNA.Furthermore,divalent ions,particularly Ca2+,facilitated the binding of ssRNA to phospholipids due to their higher binding energy and lower dissociation rate from phospholipids.Overall,our study provides valuable insights into the molecular mechanisms underlying nucleic acidphospholipid interactions,with potential implications for the nucleic acids in biotherapies,particularly in the context of lipid carriers.
文摘In this paper, we study the flocking behavior of a thermodynamic Cucker–Smale model with local velocity interactions. Using the spectral gap of a connected stochastic matrix, together with an elaborate estimate on perturbations of a linearized system, we provide a sufficient framework in terms of initial data and model parameters to guarantee flocking. Moreover, it is shown that the system achieves a consensus at an exponential rate.
基金supported by the National Research Foundation of Korea(Grant number:NRF-2023R1A2C2005864)supported by the National Research Foundation of Korea(NRF)grant funded by the Korea government(MSIT)(RS-2024-00406240)+3 种基金supported by a National Research Foundation of Korea(NRF)Grant funded by the Korean Government(MSIT)(No.2022R1A2C1003853)supported by a National Research Foundation of Korea(NRF)Grant funded by the Korean Government(MSIT)(No.RS-2023-00217661)Technology Innovation Program(RS-2022-00155961,Development of a high-efficiency drying system for carbon reduction and high-loading electrodes by a flash light source)funded by the Ministry of Trade&,Energy(MOTIE,Korea)supported by a National Research Foundation of Korea(NRF)Grant funded by the Korean Government(MSIT)(No.2022R1A2C4001497).
文摘This review provides a comprehensive overview of the progress in light-material interactions(LMIs),focusing on lasers and flash lights for energy conversion and storage applications.We discuss intricate LMI parameters such as light sources,interaction time,and fluence to elucidate their importance in material processing.In addition,this study covers various light-induced photothermal and photochemical processes ranging from melting,crystallization,and ablation to doping and synthesis,which are essential for developing energy materials and devices.Finally,we present extensive energy conversion and storage applications demonstrated by LMI technologies,including energy harvesters,sensors,capacitors,and batteries.Despite the several challenges associated with LMIs,such as complex mechanisms,and high-degrees of freedom,we believe that substantial contributions and potential for the commercialization of future energy systems can be achieved by advancing optical technologies through comprehensive academic research and multidisciplinary collaborations.
基金sponsored by the National Key R&D Program of China(2021YFA1501100)the National Natural Science Foundation of China(21832001 and 22293042)the Beijing National Laboratory for Molecular Sciences(BNLMS-CXXM-202104)。
文摘The modulation of metal-support interfacial interaction is significant but challenging in the design of high-efficiency and high-stability supported catalysts.Here,we report a synthetic strategy to upgrade Cu-CeO_(2)interfacial interaction by the pyrolysis of mixed metal-organic framework(MOF)structure.The obtained highly dispersed Cu/CeO_(2)-MOF catalyst via this strategy was used to catalyze water-gas shift reaction(WGSR),which exhibited high activity of 40.5μmolCOgcat^(-1).s^(-1)at 300℃and high stability of about 120 h.Based on comprehensive studies of electronic structure,pyrolysis strategy has significant effect on enhancing metal-support interaction and then stabilizing interfacial Cu^(+)species under reaction conditions.Abundant Cu^(+)species and generated oxygen vacancies over Cu/CeO_(2)-MOF catalyst played a key role in CO molecule activation and H2O molecule dissociation,respectively.Both collaborated closely and then promoted WGSR catalytic performance in comparison with traditio nal supported catalysts.This study shall offer a robust approach to harvest highly dispersed catalysts with finely-tuned metal-support interactions for stabilizing the most interfacial active metal species in diverse heterogeneous catalytic reactions.
基金supported by the Zhejiang Provincial Natural Science Foundation of China(LGN22C200027 and LZ23C200001).
文摘Studies showed that complexation of polyphenols with milk allergens reduced their immunogenic potential.However,the relationship between structures of polyphenols and their hypoallergenic effects on milk allergens in association with physiological and conformational changes of the complexes remain unclear.In this study,polyphenols from eight botanical sources were extracted to prepare non-covalent complexes withβ-lactoglobulin(β-LG),a major allergen in milk.The dominant phenolic compounds bound toβ-LG with a diminished allergenicity were identified to investigate their respective role on the structural and allergenic properties ofβ-LG.Extracts from Vaccinium fruits and black soybeans were found to have great inhibitory effects on the IgE-and IgG-binding abilities ofβ-LG.Among the fourteen structure-related phenolic compounds,flavonoids and tannins with larger MWs and multi-hydroxyl substituents,notably rutin,EGCG,and ellagitannins were more potent to elicit changes on the conformational structures ofβ-LG to decrease the allergenicity of complexedβ-LG.Correlation analysis further demonstrated that a destabilized secondary structure and protein depolymerization caused by polyphenol-binding were closely related to the allergenicity property of formed complexes.This study provides insights into the understanding of structure-allergenicity relationship ofβ-LG-polyphenol interactions and would benefit the development of polyphenol-fortified matrices with hypoallergenic potential.
基金supported by 973 Program of China (2013CBA01700)National Natural Science Funds (61622508, 61575032)
文摘Spin-orbit optical phenomena pertain to the wider class of electromagnetic effects originating from the interaction of the photon spin with the spatial structure and propagation characteristics of an optical wave,mediated by suitable optical media.There are many emerging photonic applications of spin-orbit interactions(SOI)of light,such as control of the optical wave propagation via the spin,enhanced optical manipulation,and generation of structured optical fields.Unfortunately,current applications are based on symmetric SOI,that is,the behaviours of polarized photons with two opposite spins are opposite,leading to the limit of spin-based multiplexers.The symmetry of SOI can be broken in our proposed metasurfaces,consisting of spatially varying birefringence,which can arbitrarily and independently build SOI for two opposite spins without reduction of optical energy usage.We obtain three kinds of dual-functional metasurfaces at visible and infrared wavelengths with high efficiency.Our concept of generation of asymmetric SOI for two spins,using anisotropic metasurfaces,will open new degrees of freedoms for building new types of spin-controlled multifunctional shared-aperture devices for the generation of complex structured optical fields.
基金the financial support of the National Basic Research Program(973 Program)(No.2012CB619600)the National Natural Science Foundation(Nos.51131004,51071100,51001071,51511130038,51501111,51471190)+1 种基金the National High-Tech R&D Program(863 Program)(No.2012AA030311)the research grant(Nos.14DZ2261200,15JC1402100,13PJ1404000,14520710100)from Shanghai government
文摘Realizing the uniform dispersion of nanocarbons such as carbon nanotube and graphene in metals, is an essential prerequisite to fully exhibit their enhancement effect in mechanical, thermal, and electrical properties of metal matrix composites(MMCs). In this work, we propose an effective method to achieve uniform distribution of nanocarbons in various metal flakes through a slurry-based method. It relies on the electrostatic interactions between the negatively charged nanocarbons and the positively charged metal flakes when mixed in slurry. For case study, flake metal powders(Al, Mg, Ti,Fe, and Cu) were positively charged in aqueous suspension by spontaneous ionization or cationic surface modification. While nanocarbons, given examples as carboxylic multi-walled carbon nanotubes, pristine single-walled carbon nanotube, and carbon nanotube–graphene oxide hybrid were negatively charged by the ionization of oxygen-containing functional groups or anionic surfactant. It was found that through the electrostatic interaction mechanism, all kinds of nanocarbons can be spontaneously and efficiently adsorbed onto the surface of various metal flakes. The development of such a versatile method would provide us great opportunities to fabricate advanced MMCs with appealing properties.
基金Project supported by the National Natural Science Foundation of China(Grant No.51602028)the Science and Technology Development Project of Jilin Province,China(Grant No.20160520114JH)+1 种基金the Youth Science Fund of Changchun University of Science and Technology,China(Grant No.XQNJJ-2017-04)the Natural Science Foundation of Tianjin City,China(Grant No.13JCYBJC16400)
文摘Using the split-step Fourier transform method, we numerically investigate the generation of breathing solitons in the propagation and interactions of Airy–Gaussian（AiG） beams in a cubic–quintic nonlinear medium in one transverse dimension. We show that the propagation of single AiG beams can generate stable breathing solitons that do not accelerate within a certain initial power range. The propagation direction of these breathing solitons can be controlled by introducing a launch angle to the incident AiG beams. When two AiG beams accelerated in opposite directions interact with each other,different breathing solitons and soliton pairs are observed by adjusting the phase shift, the beam interval, the amplitudes,and the light field distribution of the initial AiG beams.
基金supported by the National Natural Science Foundations of China(Nos.51476076,51776096)
文摘The reason for the asymmetry phenomenon of shock/boundary layer interactions(SBLI)in a completely symmetric nozzle with symmetric flow conditions is still an open question.A model for the asymmetry of nozzle flows was proposed based on the properties of fluid entrainment in the mixing layer and momentum conservation.The asymmetry model is deduced based on the nozzle flow with restricted shock separation,and is still applicable for free shock separation.Flow deflection angle at nozzle exit is deduced from this model.Steady numerical simulations are conducted to model the asymmetry of the SBLIs in a planar convergent-divergent nozzle tested by previous researchers.The obtained values of deflection angle based on the numerical results of forced symmetric nozzle flows can judge the asymmetry of flows in a nozzle at some operations.It shows that the entrainment of shear layer on the separation induced by SBLTs is one of the reasons for the asymmetry in the confined SBLIs.
基金supported by the National Natural Science Foundation of China(No.32060247)the Central Guidance on Local Science and Technology Development Fund of Gansu Province(No.22ZY2QG001).
文摘Research on the spatial patterns of tree populations is critical for understanding the structure and dynamic processes of forests.However,little is known about how the underlying drivers shape these patterns and species interactions in forest systems.In this study,spatial point pattern analysis investigated the combined eff ects of intraspecifi c interactions and environmental heterogeneity on the spatial structure and internal maintenance mechanisms of Picea crassifolia in the Qilian Mountain National Nature Reserve,China.Data were obtained from a 10.2-ha dynamic monitoring plot(DMP)and sixteen 0.04-ha elevation gradient plots(EGPs).Under complete spatial randomness,both mature trees and saplings in the DMP demonstratedlarge-scale aggregation with negative correlations.In EGPs,saplings were clustered in small mesoscales,mature trees were randomly distributed,and the interactions of saplingstrees at all elevations were not correlated.By eliminating the interference of environmental heterogeneity through the inhomogeneous Poisson process,saplings in the DMP and EGPs were clustered in small scales and trees randomly distributed.Intraspecifi c associations were negatively correlated,in the DMP and at low elevations,and no correlations in high elevations of EGPs.In the vertical scale,saplings showed a small-scale aggregation pattern with increase in elevation,and the aggregation degree fi rst decreased and then increased.The interactions of saplings-trees and saplings–saplings showed inhibitions at small scales,with the degree of inhibition gradually decreasing.Spatial patterns and associations of adults–adults did not change signifi-cantly.The results revealed that intraspecifi c interactions and environmental heterogeneity regulated the spatial patterns of P.crassifolia at small and large scales,respectively.Environmental heterogeneity might be the most decisive factor aff ecting the spatial patterns of saplings,while trees were more aff ected by intraspecifi c interactions.Moreover,competition between trees in this area could be more common than facilitation for the growth and development of individuals.
基金Project supported by the National Natural Science Foundation of China （Grant No 10375024） and the Science Foundation of Hunan Educational Committee, China
文摘The depletion interactions between two large-spheres immersed in a fluid of small spheres under unsymmetrical geometrical confinement are studied through the acceptance ratio method. The numerical results show that no matter whether the volume fraction is large or small, both the depletion potential and depletion force are affected by the presence of the two plates; the closer the two large spheres are to the plate, the larger the effects of the unsymmetrical confinements.
基金funded by the NSFC(51602193)Shanghai“Chen Guang”Project(16CG63)+2 种基金the Fundamental Research Funds for the Central Universities(WD1817002)the STFC Batteries Network(ST/R006873/1)funding from the EPSRC(EP/R023581/1,EP/P009050/1).
文摘Hydrogen is one of the most attractive renewables for future energy application,therefore it is vital to develop cost-effective and highlyefficient electrocatalysts for the hydrogen evolution reaction(HER)to promote the generation of hydrogen from mild methods.In this work,Co–Mo phosphide nanosheets with the adjustable ratio of Co and Mo were fabricated on carbon cloth by a facile hydrothermal-annealing method.Owing to the unique nanostructures,abundant active surfaces and small resistance were achieved.Excellent electrocatalytic performances are obtained,such as the small overpotential of^67.3 mV to realize a current density of 10 mA cm^(-2) and a Tafel slope of 69.9 mV dec^(-1).Rapid recovery of the current response under multistep chronoamperometry is realized and excellent stability retained after the CV test for 2000 cycles.The change of electronic states of different elements was carefully studied which suggested the optimal electrochemical performance can be realized by tuning phosphorous and metal interactions.
基金Project supported by the National Natural Science Foundation of China （Grant No 10672147） and Natural Science Foundation of Zhejiang Forestry University, China （Grant No 2006FR035）. Acknowledgments The authors are indebted to Professor Zhang J F for his helpful suggestions and fruitful discussions, and also express their sincere thanks to the editors and the anonymous referees for their constructive suggestions and kind help.
文摘Starting from the extended tanh-function method （ETM） based on the mapping method, the variable separation solutions of the （2＋1）-dimensional asymmetric Nizhnik Novikov Veselov （ANNV） system are derived. By further study, we find that these variable separation solutions are seemingly independent of but actually dependent on each other. Based on the variable separation solution and by choosing appropriate functions, some novel and interesting interactions between special solitons, such as bell-like compacton, peakon-like compacton and compacton-like semifoldon, are investigated.
