Antiferromagnetic spin fluctuation is regarded as the leading driving force for electron pairing in high-Tc superconductors.In iron-based superconductors,spin excitations at low energy range,especially the spin-resona...Antiferromagnetic spin fluctuation is regarded as the leading driving force for electron pairing in high-Tc superconductors.In iron-based superconductors,spin excitations at low energy range,especially the spin-resonance mode at ER~5kBTc,are important for understanding the superconductivity.Here,we use inelastic neutron scattering(INS)to investigate the symmetry and in-plane wave-vector dependence of low-energy spin excitations in uniaxial-strain detwinned Fe Se.The low-energy spin excitations(E<10 meV)appear mainly at Q=(±1,0)in the superconducting state(T9K)and the nematic state(T90 K),confirming the constant C_(2)rotational symmetry and ruling out the C_(4)mode at E≈3 meV reported in a prior INS study.Moreover,our results reveal an isotropic spin resonance in the superconducting state,which is consistent with the s±wave pairing symmetry.At slightly higher energy,low-energy spin excitations become highly anisotropic.The full width at half maximum of spin excitations is elongated along the transverse direction.The Q-space isotropic spin resonance and highly anisotropic low-energy spin excitations could arise from dyz intra-orbital selective Fermi surface nesting between the hole pocket aroundΓpoint and the electron pockets centered at MX point.展开更多
Typically, the unambiguous determination of the quantum numbers of nuclear states is a challenging task. Recently, it has been proposed to utilize to this aim vortex photons in the MeV energy region and, potentially, ...Typically, the unambiguous determination of the quantum numbers of nuclear states is a challenging task. Recently, it has been proposed to utilize to this aim vortex photons in the MeV energy region and, potentially, this could revolutionize nuclear spectroscopy because of the new and enhanced selectivity of this probe. Moreover, nuclei may become diagnostic tools for vortex photons. Still, some open questions have to be dealt with.Nuclei exhibit intricate excitation spectra. Indeed, not all states within these spectra are equally significant. Some are not sensitive to specific terms in the nuclear Hamiltonian or do not display novel features, so that investigating them is not helpful to enhance our overall understanding of nuclear structure. On the other hand, there are states that manifest themselves as prominent peaks, e.g., in the inelastic scattering spectra. Among the best examples are the so-called Giant Resonances that lie at energies of the order of tens of MeV [1].展开更多
Investigating the impact of microhydration on the excited-states and electronic excitation properties of biomolecules has remained one of the important yet challenging aspects of science because of the complexity of d...Investigating the impact of microhydration on the excited-states and electronic excitation properties of biomolecules has remained one of the important yet challenging aspects of science because of the complexity of developing models. However, with the advent of computational chemistry methods such as TD-DFT, many useful insights about the electronic excitation energy and excited-state nature of biomolecules can be explored. Accordingly, in our study, we have incorporated the TD-DFT/wB97XD/cc-pVTZ method to study the excited state properties of N-acetyl phenylalanine amide (NAPA-A(H<sub>2</sub>O) <sub>n</sub>) (n = 1 to 4) clusters from ground to the tenth lowest gaseous singlet excited state. We found that the C=O bond length gradually increases both in N-terminal amide and C-terminal amide after the sequential addition of water molecules because of intermolecular H-bonding and this intermolecular H-bonding becomes weaker after the sequential addition of H<sub>2</sub>O molecules. The UV absorption maxima of NAPA-A (H<sub>2</sub>O)<sub>n</sub> (n = 1 - 4) clusters consisted of two peaks that are S<sub>5</sub>←S<sub>0</sub> (1<sup>st</sup> absorption) and S<sub>6</sub>←S<sub>0</sub> (2<sup>nd</sup> absorption) excitations. The first absorption maxima were blue-shifted with the increase in oscillator strength. This means that strong H-bonds reduce the charge transfer and make clusters more rigid. On the other hand, the second absorption maxima were red-shifted with the decrease in oscillator strength. In the ECD spectra, the negative bands indicate the presence of an amide bond and L-configuration of micro hydrated NAPA-A clusters. Finally, our calculated absorption and fluorescence energy confirm that all the NAPA-A (H<sub>2</sub>O) <sub>n</sub> (n = 0 - 4) clusters revert to the ground state from the fluorescent state by emitting around 5.490 eV of light.展开更多
Hysteresis widely exists in civil structures,and dissipates the mechanical energy of systems.Research on the random vibration of hysteretic systems,however,is still insufficient,particularly when the excitation is non...Hysteresis widely exists in civil structures,and dissipates the mechanical energy of systems.Research on the random vibration of hysteretic systems,however,is still insufficient,particularly when the excitation is non-Gaussian.In this paper,the radial basis function(RBF)neural network(RBF-NN)method is adopted as a numerical method to investigate the random vibration of the Bouc-Wen hysteretic system under the Poisson white noise excitations.The solution to the reduced generalized Fokker-PlanckKolmogorov(GFPK)equation is expressed in terms of the RBF-NNs with the Gaussian activation functions,whose weights are determined by minimizing the loss function of the reduced GFPK equation residual and constraint associated with the normalization condition.A steel fiber reinforced ceramsite concrete(SFRCC)column loaded by the Poisson white noise is studied as an example to illustrate the solution process.The effects of several important parameters of both the system and the excitation on the stochastic response are evaluated,and the obtained results are compared with those obtained by the Monte Carlo simulations(MCSs).The numerical results show that the RBF-NN method can accurately predict the stationary response with a considerable high computational efficiency.展开更多
We demonstrate the flexible tunability of excitation transport in Rydberg atoms,under the interplay of controlled dissipation and interaction-induced synthetic flux.Considering a minimum four-site setup,i.e.,a triangu...We demonstrate the flexible tunability of excitation transport in Rydberg atoms,under the interplay of controlled dissipation and interaction-induced synthetic flux.Considering a minimum four-site setup,i.e.,a triangular configuration with an additional output site,we study the transport of a single excitation.展开更多
Excitation and inhibition are at the core of brain function and malfunction.To sustain the activity of neuronal networks over time and space,glutamatergic excitation is balanced by GABAergic inhibition.The equipoise o...Excitation and inhibition are at the core of brain function and malfunction.To sustain the activity of neuronal networks over time and space,glutamatergic excitation is balanced by GABAergic inhibition.The equipoise of excitation and inhibition,known as the excitation/inhibition(E/I)balance,is crucial for proper brain function.The E/I balance is highly dynamic and shifts across different brain states:wakefulness primarily augments excitatory activity,while sleep promotes a decrease in excitation and an increase in inhibition(Bridi et al.,2020).Neuronal activity during various brain states is primarily regulated by neurotransmitters(Schiemann et al.,2015),alongside non-synaptic mechanisms that operate on a slower timescale.The non-synaptic mechanisms are many,with the ionic composition of the extracellular space playing a significant role;altering extracellular ion concentrations affects sleep,arousal,electroencephalogram patterns,and behavioral states(Ding et al.,2016).展开更多
Quantum excitation is usually regarded as a transient process occurring instantaneously,leaving the underlying physics shrouded in mystery.Recent research shows that Rydberg-state excitation with ultrashort laser puls...Quantum excitation is usually regarded as a transient process occurring instantaneously,leaving the underlying physics shrouded in mystery.Recent research shows that Rydberg-state excitation with ultrashort laser pulses can be investigated and manipulated with state-of-the-art few-cycle pulses.We theoretically find that the efficiency of Rydberg state excitation can be enhanced with a short laser pulse and modulated by varying the laser intensities.We also uncover new facets of the excitation dynamics,including the launching of an electron wave packet through strong-field ionization,the re-entry of the electron into the atomic potential and the crucial step where the electron makes a U-turn,resulting in twin captures into Rydberg orbitals.By tuning the laser intensity,we show that the excitation of the Rydberg state can be coherently controlled on a sub-optical-cycle timescale.Our work paves the way toward ultrafast control and coherent manipulation of Rydberg states,thus benefiting Rydberg-state-based quantum technology.展开更多
Precisely refining the electronic structure of electrocatalysts represents a powerful approach to further optimize the electrocatalytic performance.Herein,we demonstrate an ingenious d-d orbital hybridization concept ...Precisely refining the electronic structure of electrocatalysts represents a powerful approach to further optimize the electrocatalytic performance.Herein,we demonstrate an ingenious d-d orbital hybridization concept to construct Mo-doped Co_(9)S_(8) nanorod arrays aligned on carbon cloth(CC)substrate(abbreviated as Mo-Co_(9)S_(8)@CC hereafter)as a high-efficiency bifunctional electrocatalyst toward water electrolysis.It has experimentally and theoretically validated that the 4d-3d orbital coupling between Mo dopant and Co site can effectively optimize the H_(2)O activation energy and lower H^(*)adsorption energy barrier,thereby leading to enhanced hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)activities.Thanks to the unique electronic and geometrical advantages,the optimized Mo-Co_(9)S_(8)@CC with appropriate Mo content exhibits outstanding bifunctional performance in alkaline solution,with the overpotentials of 75 and 234 mV for the delivery of a current density of 10 mA cm^(-2),small Tafel slopes of 53.8 and 39.9 mV dec~(-1)and long-term stabilities for at least 32 and 30 h for HER and OER,respectively.More impressively,a water splitting electrolylzer assembled by the self-supported Mo-Co_(9)S_(8)@CC electrode requires a low cell voltage of 1.53 V at 10 mA cm^(-2)and shows excellent stability and splendid reversibility,demonstrating a huge potential for affordable and scalable electrochemical H_(2) production.The innovational orbital hybridization strategy for electronic regulation herein provides an inspirable avenue for developing progressive electrocatalysts toward new energy systems.展开更多
Cross-sections for electronic excitation and de-excitation among the ground state and lowest-lying seven electronic excited states of carbon monoxide(CO)by low-energy electron impact are computed using the R-matrix me...Cross-sections for electronic excitation and de-excitation among the ground state and lowest-lying seven electronic excited states of carbon monoxide(CO)by low-energy electron impact are computed using the R-matrix method.The excitation cross-sections from the ground state to the electronic states a^(3)Π,a'^(3)Σ^(+)+and A^(1)Πagree with previous experimental and theoretical results.In addition,the cross-sections for the I^(1)Σ^(+)-and D^(1)Δstates of CO,which will cascade to CO a'^(3)Σ^(+)+and A^(1)Πstates,are calculated.Furthermore,in contrast to the typical increase in electronic excitation cross-sections with collision energy,the de-excitation cross-sections show a negative trend with increasing energy.展开更多
The d-d orbital coupling induced by crystal-phase engineering can effectively adjust the electronic structure of electrocatalysts,thus showing significant catalytic performance,while it has been rarely explored in ele...The d-d orbital coupling induced by crystal-phase engineering can effectively adjust the electronic structure of electrocatalysts,thus showing significant catalytic performance,while it has been rarely explored in electrochemical acetonitrile reduction reaction(ARR)to date.Herein,we successfully realize the structural transformation of Pd Cu metallic aerogels(MAs)from face-centered cubic(FCC)to body-centered cubic(BCC)through annealing treatment.Specifically,the BCC Pd Cu MAs exhibit excellent ARR performance with high ethylamine selectivity of 90.91%,Faradaic efficiency of 88.60%,yield rate of 316.0 mmol h^(-1)g^(-1)_(Pd+Cu)and long-term stability for consecutive electrolysis within 20 h at-0.55 V vs.reversible hydrogen electrode,outperforming than those of FCC Pd Cu MAs.Under the membrane electrode assembly system,BCC Pd Cu MAs also demonstrate excellent ethylamine yield rate of 389.5 mmol h^(-1)g^(-1)_(Pd+Cu).Density functional theory calculation reveals that the d-d orbital coupling in BCC Pd Cu MAs results in an evident correlation effect for the interaction of Pd and Cu sites,which boosts up the Cu sites electronic activities to enhance ARR performance.Our work opens a new route to develop efficient ARR electrocatalysts from the perspective of crystalline structure transformation.展开更多
The SiS molecule,which plays a significant role in space,has attracted a great deal of attention for many years.Due to complex interactions among its low-lying electronic states,precise information regarding the molec...The SiS molecule,which plays a significant role in space,has attracted a great deal of attention for many years.Due to complex interactions among its low-lying electronic states,precise information regarding the molecular structure of SiS is limited.To obtain accurate information about the structure of its excited states,the high-precision multireference configuration interaction(MRCI)method has been utilized.This method is used to calculate the potential energy curves(PECs)of the 18Λ–S states corresponding to the lowest dissociation limit of SiS.The core–valence correlation effect,Davidson’s correction and the scalar relativistic effect are also included to guarantee the precision of the MRCI calculation.Based on the calculated PECs,the spectroscopic constants of quasi-bound and bound electronic states are calculated and they are in accordance with previous experimental results.The transition dipole moments(TDMs)and dipole moments(DMs)are determined by the MRCI method.In addition,the abrupt variations of the DMs for the 1^(5)Σ^(+)and 2^(5)Σ^(+)states at the avoided crossing point are attributed to the variation of the electronic configuration.The opacity of SiS at a pressure of 100 atms is presented across a series of temperatures.With increasing temperature,the expanding population of excited states blurs the band boundaries.展开更多
Manganese-based perovskite is popular for research on ferromagnetic materials,and its spectroscopic studies are essential for understanding its electronic structure,dielectric,electrical,and magnetic properties.In thi...Manganese-based perovskite is popular for research on ferromagnetic materials,and its spectroscopic studies are essential for understanding its electronic structure,dielectric,electrical,and magnetic properties.In this paper,the M-edge spectra of La ions and the M-edge,L-edge,and K-edge spectra of Mn ions in LaMnO3 are calculated by considering both the free-ion multiplet calculation and the crystal field effects.We analyze spectral shapes,identify peak origins,and estimate the oxidation states of La and Mn ions in LaMnO3 theoretically.It is concluded that La ions in LaMnO3 predominantly exist in the trivalent state,while Mn ions exist primarily in the trivalent state with a minor presence of tetravalent ions.Furthermore,the calculated spectra are in better conformity with the experimental spectra when the proportion of Mn3+is 90%and Mn4+is 10%.This article enhances our comprehension of the oxidation states of La and Mn within the crystal and also provides a valuable guidance for spectroscopic investigations of other manganates.展开更多
With the rapid development of large megawatt wind turbines,the operation environment of wind turbine towers(WTTs)has become increasingly complex.In particular,seismic excitation can create a resonance response and cau...With the rapid development of large megawatt wind turbines,the operation environment of wind turbine towers(WTTs)has become increasingly complex.In particular,seismic excitation can create a resonance response and cause excessive vibration of the WTT.To investigate the vibration attenuation performance of the WTT under seismic excitations,a novel passive vibration control device,called a prestressed tuned mass damper(PS-TMD),is presented in this study.First,a mathematical model is established based on structural dynamics under seismic excitation.Then,the mathematical analytical expression of the dynamic coefficient is deduced,and the parameter design method is obtained by system tuning optimization.Next,based on a theoretical analysis and parameter design,the numerical results showed that the PS-TMD was able to effectively mitigate the resonance under the harmonic basal acceleration.Finally,the time-history analysis method is used to verify the effectiveness of the traditional pendulum tuned mass damper(PTMD)and the novel PS-TMD device,and the results indicate that the vibration attenuation performance of the PS-TMD is better than the PTMD.In addition,the PS-TMD avoids the nonlinear effect due to the large oscillation angle,and has the potential to dissipate hysteretic energy under seismic excitation.展开更多
The auto-parametric resonance of a continuous-beam bridge model subjected to a two-point periodic excitation is experimentally and numerically investigated in this study.An auto-parametric resonance experiment of the ...The auto-parametric resonance of a continuous-beam bridge model subjected to a two-point periodic excitation is experimentally and numerically investigated in this study.An auto-parametric resonance experiment of the test model is conducted to observe and measure the auto-parametric resonance of a continuous beam under a two-point excitation on columns.The parametric vibration equation is established for the test model using the finite-element method.The auto-parametric resonance stability of the structure is analyzed by using Newmark's method and the energy-growth exponent method.The effects of the phase difference of the two-point excitation on the stability boundaries of auto-parametric resonance are studied for the test model.Compared with the experiment,the numerical instability predictions of auto-parametric resonance are consistent with the test phenomena,and the numerical stability boundaries of auto-parametric resonance agree with the experimental ones.For a continuous beam bridge,when the ratio of multipoint excitation frequency(applied to the columns)to natural frequency of the continuous girder is approximately equal to 2,the continuous beam may undergo a strong auto-parametric resonance.Combined with the present experiment and analysis,a hypothesis of Volgograd Bridge's serpentine vibration is discussed.展开更多
基金Beijing Normal University was supported by the Fundamental Research Funds for the Central Universitiesthe National Key Projects for Research and Development of China(No.2021YFA1400400)+1 种基金the National Natural Science Foundation of China(Grant Nos.12174029 and 11922402)the neutron beamtimes from J-PARC(Proposal No.2019A0002)。
文摘Antiferromagnetic spin fluctuation is regarded as the leading driving force for electron pairing in high-Tc superconductors.In iron-based superconductors,spin excitations at low energy range,especially the spin-resonance mode at ER~5kBTc,are important for understanding the superconductivity.Here,we use inelastic neutron scattering(INS)to investigate the symmetry and in-plane wave-vector dependence of low-energy spin excitations in uniaxial-strain detwinned Fe Se.The low-energy spin excitations(E<10 meV)appear mainly at Q=(±1,0)in the superconducting state(T9K)and the nematic state(T90 K),confirming the constant C_(2)rotational symmetry and ruling out the C_(4)mode at E≈3 meV reported in a prior INS study.Moreover,our results reveal an isotropic spin resonance in the superconducting state,which is consistent with the s±wave pairing symmetry.At slightly higher energy,low-energy spin excitations become highly anisotropic.The full width at half maximum of spin excitations is elongated along the transverse direction.The Q-space isotropic spin resonance and highly anisotropic low-energy spin excitations could arise from dyz intra-orbital selective Fermi surface nesting between the hole pocket aroundΓpoint and the electron pockets centered at MX point.
文摘Typically, the unambiguous determination of the quantum numbers of nuclear states is a challenging task. Recently, it has been proposed to utilize to this aim vortex photons in the MeV energy region and, potentially, this could revolutionize nuclear spectroscopy because of the new and enhanced selectivity of this probe. Moreover, nuclei may become diagnostic tools for vortex photons. Still, some open questions have to be dealt with.Nuclei exhibit intricate excitation spectra. Indeed, not all states within these spectra are equally significant. Some are not sensitive to specific terms in the nuclear Hamiltonian or do not display novel features, so that investigating them is not helpful to enhance our overall understanding of nuclear structure. On the other hand, there are states that manifest themselves as prominent peaks, e.g., in the inelastic scattering spectra. Among the best examples are the so-called Giant Resonances that lie at energies of the order of tens of MeV [1].
文摘Investigating the impact of microhydration on the excited-states and electronic excitation properties of biomolecules has remained one of the important yet challenging aspects of science because of the complexity of developing models. However, with the advent of computational chemistry methods such as TD-DFT, many useful insights about the electronic excitation energy and excited-state nature of biomolecules can be explored. Accordingly, in our study, we have incorporated the TD-DFT/wB97XD/cc-pVTZ method to study the excited state properties of N-acetyl phenylalanine amide (NAPA-A(H<sub>2</sub>O) <sub>n</sub>) (n = 1 to 4) clusters from ground to the tenth lowest gaseous singlet excited state. We found that the C=O bond length gradually increases both in N-terminal amide and C-terminal amide after the sequential addition of water molecules because of intermolecular H-bonding and this intermolecular H-bonding becomes weaker after the sequential addition of H<sub>2</sub>O molecules. The UV absorption maxima of NAPA-A (H<sub>2</sub>O)<sub>n</sub> (n = 1 - 4) clusters consisted of two peaks that are S<sub>5</sub>←S<sub>0</sub> (1<sup>st</sup> absorption) and S<sub>6</sub>←S<sub>0</sub> (2<sup>nd</sup> absorption) excitations. The first absorption maxima were blue-shifted with the increase in oscillator strength. This means that strong H-bonds reduce the charge transfer and make clusters more rigid. On the other hand, the second absorption maxima were red-shifted with the decrease in oscillator strength. In the ECD spectra, the negative bands indicate the presence of an amide bond and L-configuration of micro hydrated NAPA-A clusters. Finally, our calculated absorption and fluorescence energy confirm that all the NAPA-A (H<sub>2</sub>O) <sub>n</sub> (n = 0 - 4) clusters revert to the ground state from the fluorescent state by emitting around 5.490 eV of light.
基金the National Natural Science Foundation of China(No.12072118)the Natural Science Funds for Distinguished Young Scholar of Fujian Province of China(No.2021J06024)the Project for Youth Innovation Fund of Xiamen of China(No.3502Z20206005)。
文摘Hysteresis widely exists in civil structures,and dissipates the mechanical energy of systems.Research on the random vibration of hysteretic systems,however,is still insufficient,particularly when the excitation is non-Gaussian.In this paper,the radial basis function(RBF)neural network(RBF-NN)method is adopted as a numerical method to investigate the random vibration of the Bouc-Wen hysteretic system under the Poisson white noise excitations.The solution to the reduced generalized Fokker-PlanckKolmogorov(GFPK)equation is expressed in terms of the RBF-NNs with the Gaussian activation functions,whose weights are determined by minimizing the loss function of the reduced GFPK equation residual and constraint associated with the normalization condition.A steel fiber reinforced ceramsite concrete(SFRCC)column loaded by the Poisson white noise is studied as an example to illustrate the solution process.The effects of several important parameters of both the system and the excitation on the stochastic response are evaluated,and the obtained results are compared with those obtained by the Monte Carlo simulations(MCSs).The numerical results show that the RBF-NN method can accurately predict the stationary response with a considerable high computational efficiency.
基金supported by the National Natural Science Foundation of China(Grant Nos.11974331 and 12374479)。
文摘We demonstrate the flexible tunability of excitation transport in Rydberg atoms,under the interplay of controlled dissipation and interaction-induced synthetic flux.Considering a minimum four-site setup,i.e.,a triangular configuration with an additional output site,we study the transport of a single excitation.
文摘Excitation and inhibition are at the core of brain function and malfunction.To sustain the activity of neuronal networks over time and space,glutamatergic excitation is balanced by GABAergic inhibition.The equipoise of excitation and inhibition,known as the excitation/inhibition(E/I)balance,is crucial for proper brain function.The E/I balance is highly dynamic and shifts across different brain states:wakefulness primarily augments excitatory activity,while sleep promotes a decrease in excitation and an increase in inhibition(Bridi et al.,2020).Neuronal activity during various brain states is primarily regulated by neurotransmitters(Schiemann et al.,2015),alongside non-synaptic mechanisms that operate on a slower timescale.The non-synaptic mechanisms are many,with the ionic composition of the extracellular space playing a significant role;altering extracellular ion concentrations affects sleep,arousal,electroencephalogram patterns,and behavioral states(Ding et al.,2016).
基金supported by the National Key Research and Development Program of China(Grant No.2019YFA0307703)the National Natural Science Foundation of China(Grant Nos.12234020,11874066,12274461,and 11974426)the Science and Technology Innovation Program of Hunan Province(Grant No.2022RC1193).
文摘Quantum excitation is usually regarded as a transient process occurring instantaneously,leaving the underlying physics shrouded in mystery.Recent research shows that Rydberg-state excitation with ultrashort laser pulses can be investigated and manipulated with state-of-the-art few-cycle pulses.We theoretically find that the efficiency of Rydberg state excitation can be enhanced with a short laser pulse and modulated by varying the laser intensities.We also uncover new facets of the excitation dynamics,including the launching of an electron wave packet through strong-field ionization,the re-entry of the electron into the atomic potential and the crucial step where the electron makes a U-turn,resulting in twin captures into Rydberg orbitals.By tuning the laser intensity,we show that the excitation of the Rydberg state can be coherently controlled on a sub-optical-cycle timescale.Our work paves the way toward ultrafast control and coherent manipulation of Rydberg states,thus benefiting Rydberg-state-based quantum technology.
基金financially supported by the National Natural Science Foundation of China(21972068,22072067,22232004)the High-level Talents Project of Jinling Institute of Technology(jit-b-202164)。
文摘Precisely refining the electronic structure of electrocatalysts represents a powerful approach to further optimize the electrocatalytic performance.Herein,we demonstrate an ingenious d-d orbital hybridization concept to construct Mo-doped Co_(9)S_(8) nanorod arrays aligned on carbon cloth(CC)substrate(abbreviated as Mo-Co_(9)S_(8)@CC hereafter)as a high-efficiency bifunctional electrocatalyst toward water electrolysis.It has experimentally and theoretically validated that the 4d-3d orbital coupling between Mo dopant and Co site can effectively optimize the H_(2)O activation energy and lower H^(*)adsorption energy barrier,thereby leading to enhanced hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)activities.Thanks to the unique electronic and geometrical advantages,the optimized Mo-Co_(9)S_(8)@CC with appropriate Mo content exhibits outstanding bifunctional performance in alkaline solution,with the overpotentials of 75 and 234 mV for the delivery of a current density of 10 mA cm^(-2),small Tafel slopes of 53.8 and 39.9 mV dec~(-1)and long-term stabilities for at least 32 and 30 h for HER and OER,respectively.More impressively,a water splitting electrolylzer assembled by the self-supported Mo-Co_(9)S_(8)@CC electrode requires a low cell voltage of 1.53 V at 10 mA cm^(-2)and shows excellent stability and splendid reversibility,demonstrating a huge potential for affordable and scalable electrochemical H_(2) production.The innovational orbital hybridization strategy for electronic regulation herein provides an inspirable avenue for developing progressive electrocatalysts toward new energy systems.
基金Project supported by the National Natural Science Foundation of China (Grant No.11974253)。
文摘Cross-sections for electronic excitation and de-excitation among the ground state and lowest-lying seven electronic excited states of carbon monoxide(CO)by low-energy electron impact are computed using the R-matrix method.The excitation cross-sections from the ground state to the electronic states a^(3)Π,a'^(3)Σ^(+)+and A^(1)Πagree with previous experimental and theoretical results.In addition,the cross-sections for the I^(1)Σ^(+)-and D^(1)Δstates of CO,which will cascade to CO a'^(3)Σ^(+)+and A^(1)Πstates,are calculated.Furthermore,in contrast to the typical increase in electronic excitation cross-sections with collision energy,the de-excitation cross-sections show a negative trend with increasing energy.
基金financially supported by the National Natural Science Foundation of China(Grant Nos.52161135302,22105087)the Postdoctoral Research Foundation of China(Grant No.2022M721360)the Natural Science Foundation of Jiangsu Province(Grant No.BK20210446)。
文摘The d-d orbital coupling induced by crystal-phase engineering can effectively adjust the electronic structure of electrocatalysts,thus showing significant catalytic performance,while it has been rarely explored in electrochemical acetonitrile reduction reaction(ARR)to date.Herein,we successfully realize the structural transformation of Pd Cu metallic aerogels(MAs)from face-centered cubic(FCC)to body-centered cubic(BCC)through annealing treatment.Specifically,the BCC Pd Cu MAs exhibit excellent ARR performance with high ethylamine selectivity of 90.91%,Faradaic efficiency of 88.60%,yield rate of 316.0 mmol h^(-1)g^(-1)_(Pd+Cu)and long-term stability for consecutive electrolysis within 20 h at-0.55 V vs.reversible hydrogen electrode,outperforming than those of FCC Pd Cu MAs.Under the membrane electrode assembly system,BCC Pd Cu MAs also demonstrate excellent ethylamine yield rate of 389.5 mmol h^(-1)g^(-1)_(Pd+Cu).Density functional theory calculation reveals that the d-d orbital coupling in BCC Pd Cu MAs results in an evident correlation effect for the interaction of Pd and Cu sites,which boosts up the Cu sites electronic activities to enhance ARR performance.Our work opens a new route to develop efficient ARR electrocatalysts from the perspective of crystalline structure transformation.
基金Project supported by the Natural Science Foundation of Heilongjiang Province,China(Grant No.LH2022A026)the National Key Research and Development Program of China(Grant No.2022YFA1602500)+2 种基金the National Natural Science Foundation of China(Grant No.11934004)Fundamental Research Funds in Heilongjiang Province Universities,China(Grant No.145109309)Foundation of National Key Laboratory of Computational Physics(Grant No.6142A05QN22006)。
文摘The SiS molecule,which plays a significant role in space,has attracted a great deal of attention for many years.Due to complex interactions among its low-lying electronic states,precise information regarding the molecular structure of SiS is limited.To obtain accurate information about the structure of its excited states,the high-precision multireference configuration interaction(MRCI)method has been utilized.This method is used to calculate the potential energy curves(PECs)of the 18Λ–S states corresponding to the lowest dissociation limit of SiS.The core–valence correlation effect,Davidson’s correction and the scalar relativistic effect are also included to guarantee the precision of the MRCI calculation.Based on the calculated PECs,the spectroscopic constants of quasi-bound and bound electronic states are calculated and they are in accordance with previous experimental results.The transition dipole moments(TDMs)and dipole moments(DMs)are determined by the MRCI method.In addition,the abrupt variations of the DMs for the 1^(5)Σ^(+)and 2^(5)Σ^(+)states at the avoided crossing point are attributed to the variation of the electronic configuration.The opacity of SiS at a pressure of 100 atms is presented across a series of temperatures.With increasing temperature,the expanding population of excited states blurs the band boundaries.
基金Project supported by the National Natural Science Foundation of China(Grant No.11974253).
文摘Manganese-based perovskite is popular for research on ferromagnetic materials,and its spectroscopic studies are essential for understanding its electronic structure,dielectric,electrical,and magnetic properties.In this paper,the M-edge spectra of La ions and the M-edge,L-edge,and K-edge spectra of Mn ions in LaMnO3 are calculated by considering both the free-ion multiplet calculation and the crystal field effects.We analyze spectral shapes,identify peak origins,and estimate the oxidation states of La and Mn ions in LaMnO3 theoretically.It is concluded that La ions in LaMnO3 predominantly exist in the trivalent state,while Mn ions exist primarily in the trivalent state with a minor presence of tetravalent ions.Furthermore,the calculated spectra are in better conformity with the experimental spectra when the proportion of Mn3+is 90%and Mn4+is 10%.This article enhances our comprehension of the oxidation states of La and Mn within the crystal and also provides a valuable guidance for spectroscopic investigations of other manganates.
基金Fundamental Research Funds for the National Natural Science Foundation of China under Grant No.52078084the Natural Science Foundation of Chongqing (cstc2021jcyj-msxmX0623)+2 种基金the 111 project of the Ministry of Educationthe Bureau of Foreign Experts of China under Grant No.B18062China Postdoctoral Science Foundation under Grant No.2021M690838。
文摘With the rapid development of large megawatt wind turbines,the operation environment of wind turbine towers(WTTs)has become increasingly complex.In particular,seismic excitation can create a resonance response and cause excessive vibration of the WTT.To investigate the vibration attenuation performance of the WTT under seismic excitations,a novel passive vibration control device,called a prestressed tuned mass damper(PS-TMD),is presented in this study.First,a mathematical model is established based on structural dynamics under seismic excitation.Then,the mathematical analytical expression of the dynamic coefficient is deduced,and the parameter design method is obtained by system tuning optimization.Next,based on a theoretical analysis and parameter design,the numerical results showed that the PS-TMD was able to effectively mitigate the resonance under the harmonic basal acceleration.Finally,the time-history analysis method is used to verify the effectiveness of the traditional pendulum tuned mass damper(PTMD)and the novel PS-TMD device,and the results indicate that the vibration attenuation performance of the PS-TMD is better than the PTMD.In addition,the PS-TMD avoids the nonlinear effect due to the large oscillation angle,and has the potential to dissipate hysteretic energy under seismic excitation.
基金National Natural Science Foundation of China under Grant No.51879191。
文摘The auto-parametric resonance of a continuous-beam bridge model subjected to a two-point periodic excitation is experimentally and numerically investigated in this study.An auto-parametric resonance experiment of the test model is conducted to observe and measure the auto-parametric resonance of a continuous beam under a two-point excitation on columns.The parametric vibration equation is established for the test model using the finite-element method.The auto-parametric resonance stability of the structure is analyzed by using Newmark's method and the energy-growth exponent method.The effects of the phase difference of the two-point excitation on the stability boundaries of auto-parametric resonance are studied for the test model.Compared with the experiment,the numerical instability predictions of auto-parametric resonance are consistent with the test phenomena,and the numerical stability boundaries of auto-parametric resonance agree with the experimental ones.For a continuous beam bridge,when the ratio of multipoint excitation frequency(applied to the columns)to natural frequency of the continuous girder is approximately equal to 2,the continuous beam may undergo a strong auto-parametric resonance.Combined with the present experiment and analysis,a hypothesis of Volgograd Bridge's serpentine vibration is discussed.
