The integration of machine learning and electrocatalysis presents nota ble advancements in designing and predicting the performance of chiral materials for hydrogen evolution reactions(HER).This study utilizes theoret...The integration of machine learning and electrocatalysis presents nota ble advancements in designing and predicting the performance of chiral materials for hydrogen evolution reactions(HER).This study utilizes theoretical calculations and machine learning techniques to assess the HER performance of both chiral and achiral M-N-SWCNTs(M=In,Bi,and Sb)single-atom catalysts(SACs).The stability preferences of metal atoms are dependent on chirality when interacting with chiral SWCNTs.The HER activity of the right-handed In-N-SWCNT is 5.71 times greater than its achiral counterpart,whereas the left-handed In-N-SWCNT exhibits a 5.12-fold enhancement.The calculated hydrogen adsorption free energy for the right-handed In-N-SWCNT reaches as low as-0.02 eV.This enhancement is attributed to the symmetry breaking in spin density distribution,transitioning from C_(2V)in achiral SACs to C_(2)in chiral SACs,which facilitates active site transfer and enhances local spin density.Right-handed M-N-SWCNTs exhibit superiorα-electron separation and transport efficiency relative to left-handed variants,owing to the chiral induced spin selectivity(CISS)effect,with spin-upα-electron density reaching 3.43×10^(-3)e/Bohr^(3)at active sites.Machine learning provides deeper insights,revealing that the interplay of weak spatial electronic effects and appropriate curvature-chirality effects significantly enhances HER performance.A weaker spatial electronic effect correlates with higher HER activity,larger exchange current density,and higher turnover frequency.The curvature-chirality effect undersco res the influence of intrinsic structures on HER performance.These findings offer critical insights into the role of chirality in electrocatalysis and propose innovative approaches for optimizing HER through chirality.展开更多
Elastic neutron diffraction measurements were performed on single crystals to study the ground state below the mysterious exotic transition temperature 0.86 K. An antiferromagnetic order with a tiny moment of 0.027 μ...Elastic neutron diffraction measurements were performed on single crystals to study the ground state below the mysterious exotic transition temperature 0.86 K. An antiferromagnetic order with a tiny moment of 0.027 μB per formula is formed as the ground state for CeOs4Sb12 below the transition point. Our neutron data gives the evidence of spin density wave state for CeOs4Sb12 in this work.展开更多
A supramolecular 1D ferromagnetic system was studied experimentally as well as theoretically.Hybrid density functional theory（DFT） calculations were based on the X-ray analysis.The results of DFT calculations and Mc...A supramolecular 1D ferromagnetic system was studied experimentally as well as theoretically.Hybrid density functional theory（DFT） calculations were based on the X-ray analysis.The results of DFT calculations and McConnell mechanism have contributed to the understanding of the factors governing the exchange coupling of magnetism in the crystal packing.Both the experimental evidence and theoretical calculation indicate that spin density in 2-iodo nitronyl nitroxide（INN） radicals confirms 1D ferromagnetic chain with inter-chain antiferromagnetic interaction.展开更多
The recent discovery of superconductivity in La_(3)Ni_(2)O_(7-δ)with a transition temperature Tc close to 80 K at high pressures has attracted significant attention,due particularly to a possible density wave(DW)tran...The recent discovery of superconductivity in La_(3)Ni_(2)O_(7-δ)with a transition temperature Tc close to 80 K at high pressures has attracted significant attention,due particularly to a possible density wave(DW)transition occurring near the superconducting dome.Identifying the type of DW order is crucial for understanding the origin of superconductivity in this system.However,owing to the presence of La4Ni3O10 and other intergrowth phases in La_(3)Ni_(2)O_(7-δ)samples,extracting the intrinsic information from the La_(3)Ni_(2)O_(7) phase is challenging.In this study,we employed ^(139)La nuclear quadrupole resonance(NQR)measurements to eliminate the influence of other structural phases in the sample and obtain microscopic insights into the DW transition in La_(3)Ni_(2)O_(7-δ).Below the DW transition temperature T_(DW)∼153 K,we observe a distinct splitting in the±5/2↔±7/2 transition of the NQR resonance peak at the La(2)site,while only a line broadening is seen in the±3/2↔±5/2 transition peak.Through further analysis of the spectra,we show that the line splitting is due to a unidirectional charge modulation.A magnetic line broadening is also observed below T_(DW),accompanied by a large enhancement of the spin-lattice relaxation rate,indicating the formation of magnetically ordered moments in the DW state.Our results suggest a simultaneous formation of charge-and spin-density wave orders in La_(3)Ni_(2)O_(7-δ),thereby offering critical insights into the electronic correlations in Ni-based superconductors.展开更多
The evolution of the spin density vectors(SDVs) is studied in a strongly focused composite field. It is found that the SDVs can be spiral along the propagation axis, and they are perpendicular to the ysdirection on th...The evolution of the spin density vectors(SDVs) is studied in a strongly focused composite field. It is found that the SDVs can be spiral along the propagation axis, and they are perpendicular to the ysdirection on the ysaxis. This behavior is governed by the Gouy phase difference between the field polarization components. The 60° rotation of the spatial distribution of the transverse SDVs is also generated, which is found to be controlled by the Gouy phase difference between the field orbital angular momentum modes. Additionally, the spin density singularities are observed in the evolution of the SDVs.展开更多
In order to shed light upon the nature and mechanism of 4f-3d magnetic exchange interactions, a series of binuclear complexes of lanthanide（3＋） and chromium（3＋） with the general formula [Ln（L）5（H2O）2Cr（CN）...In order to shed light upon the nature and mechanism of 4f-3d magnetic exchange interactions, a series of binuclear complexes of lanthanide（3＋） and chromium（3＋） with the general formula [Ln（L）5（H2O）2Cr（CN）6]·mL· nH2O （Ln=La （1）, Ce （2）, Pr （3）, Nd （4）; x=5, y=2, m=1 or 2, n=2 or 2.5; L=2-pyrrolidinone） and [Ln（L）4（H2O）3Cr（CN）6] ·nH2O （Ln=Sm （5）, Eu （6）, Gd （7）, Tb （8）, Dy （9）, Er （10）; x=4, y=3, m=0, n= 1.5 or 2.0; L=2-pyrrolidinone） were prepared and the X-ray crystal structures of complexes 2, 6 and 7 were determined. All the compounds consist of a Ln-CN-Cr unit, in which Ln^3＋ in a square antiprism environment is bridged to an octahedral coordinated Cr^3＋ ion through a cyano group. The magnetic properties of the complexes 3 and 6-10 show an overall antiferromagnetic behavior. The fitting to the experimental magnetic susceptibilities of 7 give g= 1.98, J=0.40 cm^-1, zJ＇= -0.21 cm^-1 on the basis of a binuclear spin system （Scd=7/2, Scr=3/2）, revealing an intra-molecular Gd^3＋-Cr^3＋ ferromagnetic interaction and an inter-molecular antiferromagnetic interaction. For 7 the calculation of quantum chemical density functional theory （DFT）, combined with the broken symmetry approach, showed that the calculated spin coupling constant was 20.3 cm^-1, supporting the observation of weak ferromagnetic intra-molecular interaction in 7. The spin density distributions of 7 in both the high spin ground state and the broken symmetry state were obtained, and the spin coupling mechanism between Gd^3＋ and Cr^3＋ was discussed.展开更多
We investigate the spin density matrix of Ω− in the Cartesian coordinate system of baryon-antibaryon pairs produced in e+e−annihilation.Using the helicity formalism of Jacob and Wick,we derive the expression for the ...We investigate the spin density matrix of Ω− in the Cartesian coordinate system of baryon-antibaryon pairs produced in e+e−annihilation.Using the helicity formalism of Jacob and Wick,we derive the expression for the spin-3/2 density matrices.Our analysis is based on the angular distribution of the process e+e−→ψ(3686)→Ω−Ω¯^(+ )in the BESIII experiment.By decomposing the polarization state of Ω− particles along different coordinate axes,we examine the polarization dependence of the cross-section.Our results demonstrate that Ω− particles exhibit varying degrees of tensor polarization along the x-,y-,and z-axes,as well as weak vector polarization and rank-3 tensor polarization along the y-axis.To the best of our knowledge,this is the first study to calculate the polarization dependence of the cross-section distributions for the annihilation process e+e−→Ω−Ω¯^(+).Our theoretical predictions are in good agreement with the experimental measurements.展开更多
Recently,a signature of high-temperature superconductivity above the liquid nitrogen temperature(77 K)was reported for La_(3)Ni_(2)O_(7−δ) under pressure.This finding immediately stimulated intense interest in the po...Recently,a signature of high-temperature superconductivity above the liquid nitrogen temperature(77 K)was reported for La_(3)Ni_(2)O_(7−δ) under pressure.This finding immediately stimulated intense interest in the possible mechanism of high-Tc superconductivity in double-layer nickelates.Notably,the pressure-dependent phase diagram inferred from transport measurements indicates that the superconductivity under high pressure emerges from the suppression of density-wave-like order at ambient pressure,which is similar to high-temperature superconductors.Therefore,clarifying the exact nature of the density-wave-like transition is important for determining the superconducting mechanism in double-layer nickelates.Here,nuclear magnetic resonance(NMR)spectroscopy of 139La nuclei was performed to study the density-wave-like transition in a single crystal of La_(3)Ni_(2)O_(7−δ.)At high temperatures,two sets of sharp 139La NMR peaks are clearly distinguishable from a broad background signals,which are ascribed to La(1)sites from two bilayer Ruddlesden-Popper phases with different oxygen vacancyδ.As the temperature decreases,the temperature-dependent^(139)La NMR spectra and nuclear spin-lattice relaxation rate(1/T_(1))for both La(1)sites provide evidence of spin-density-wave(SDW)ordering below the transition temperature(T_(SDW)),which is approximately 150 K.The anisotropic splitting in the NMR spectra suggests the formation of a possible double spin stripe with magnetic moments aligned along the c-axis.Furthermore,we studied the pressure-dependent SDW transition up to∼2.7 GPa.Surprisingly,the TSDW inferred from NMR measurements of both La(1)sites increases with increasing pressure,which is opposite to the results from previous transport measurements under pressure and suggests an intriguing phase diagram between superconductivity and SDW.In contrast,the present^(139)La NMR is insensitive to the possible charge-density-wave(CDW)order in the Ni-O planes.All these results will be helpful for building a connection between superconductivity and magnetic interactions in double-layer nickelates.展开更多
UiO-66-H MOFs can effectively catalyze the direct selective oxidation of methane(DSOM)to high value-added oxygenates under mild conditions.However,UiO-66-NH_(2)with benzene-1,4-dicarboxylate(NH_(2)-BDC)ligand modifyin...UiO-66-H MOFs can effectively catalyze the direct selective oxidation of methane(DSOM)to high value-added oxygenates under mild conditions.However,UiO-66-NH_(2)with benzene-1,4-dicarboxylate(NH_(2)-BDC)ligand modifying the Zr-oxo nodes exhibits relatively inferior catalytic performance for DSOM.Here,a combination of density functional theory(DFT)calculations and experiments was employed to explore the underlying reasons for the limited catalytic activity of UiO-66-NH_(2).The results indicate that the methane hydroxylation performance of UiO-66-NH_(2)is almost unaffected by the increase of·OH concentration.This is attributed to the formation of substantial non-covalent hydrogen bonds between the oxygen atoms of oxygenic species on the Zr-oxo nodes and the hydrogen atoms of-NH_(2)groups,which diminishes the spin density distribution on the active sites of(·OH)m/UiO-66-NH_(2),leading to minimal change of the adsorption energy of CH_(4).Additionally,the calculated adsorption energies(Eads)of CH_(4)exhibit a linear relationship with the catalytic activity of UiO-66-NH_(2)for DSOM reaction.展开更多
In quasi-one-dimensional(q1D) quantum antiferromagnets, the complicated interplay of intrachain and interchain exchange couplings may give rise to rich phenomena. Motivated by recent progress on field-induced phase tr...In quasi-one-dimensional(q1D) quantum antiferromagnets, the complicated interplay of intrachain and interchain exchange couplings may give rise to rich phenomena. Motivated by recent progress on field-induced phase transitions in the q1D antiferromagnetic(AFM) compound YbAlO3, we study the phase diagram of spin-1/2 Heisenberg chains with Ising anisotropic interchain couplings under a longitudinal magnetic field via large-scale quantum Monte Carlo simulations,and investigate the role of the spin anisotropy of the interchain coupling on the ground state of the system. We find that the Ising anisotropy of the interchain coupling can significantly enhance the longitudinal spin correlations and drive the system to an incommensurate AFM phase at intermediate magnetic fields, which is understood as a longitudinal spin density wave(LSDW). With increasing field, the ground state changes to a canted AFM order with transverse spin correlations. We further provide a global phase diagram showing how the competition between the LSDW and the canted AFM states is tuned by the Ising anisotropy of the interchain coupling.展开更多
The spin transport properties of S–Au–S junction and Au–Au–Au junction between Au nanowires are investigated with density functional theory and the non-equilibrium Green＇s function. We mainly focus on the spin re...The spin transport properties of S–Au–S junction and Au–Au–Au junction between Au nanowires are investigated with density functional theory and the non-equilibrium Green＇s function. We mainly focus on the spin resonance transport properties of the center Au atom. The breaking of chemical bonds between anchor atoms and center Au atom significantly influences their spin transmission characteristics. We find the 0.8 eV orbital energy shift between anchor S atoms and the center Au atom can well protect the spin state stored in the S–Au–S junction and efficiently extract its spin state to the current by spin resonance mechanism, while the spin interaction of itinerant electrons and the valence electron of the center Au atom in the Au–Au–Au junction can extract the current spin information into the center Au atom. Fermi energy drift and bias-dependent spin filtering properties of the Au–Au–Au junction may transform information between distance, bias,and electron spin. Those unique properties make them potential candidates for a logical nanocircuit.展开更多
Development of a high-performance bifunctional catalyst is essential for the actual implementation of zinc-air batteries in practical applications.Herein,a bifunctional cathode of Co_(3)S_(4)/FeS heterogeneous nanopar...Development of a high-performance bifunctional catalyst is essential for the actual implementation of zinc-air batteries in practical applications.Herein,a bifunctional cathode of Co_(3)S_(4)/FeS heterogeneous nanoparticles embedded in Co/Fe single-atom-loaded nitrogen-doped carbon nanosheets is designed.Cobalt-iron sulfides and single atomic sites with Co-N_(4)/Fe-N_(4)configurations are confirmed to coexist on the carbon matrix by EXAFS spectroscopy.3D self-supported super-hydrophobic multiphase composite cathode provides abundant active sites and facilitates gas–liquid-solid three-phase interface reactions,resulting in excellent electrocatalytic activity and batteries performance,i.e.,an OER overpotential(η_(10))of 260 mV,a half-wave potential(E_(1/2))of 0.872 V for ORR,aΔE of 0.618 V,and a discharge power density of 170 mW cm^(−2),a specific capacity of 816.3 mAh g^(−1).DFT analysis shows multiphase coupling of sulfide heterojunction through single-atomic metal doped carbon nanosheets reduces offset on center of electronic density of states before and after oxygen adsorption,and spin density of adsorbed oxygen with same spin orientation,leading to weakened charge/spin interactions between adsorbed oxygen and substrate,and a lowered oxygen adsorption energy to accelerate OER/ORR.展开更多
Research on nickel-based superconductors has progressed from infinite-layer LaNiO_(2) to finite-layer La_(6)Ni_(5)O_(12),and most recently to the Ruddlesden-Popper phase La_(3)Ni_(2)O_(7),which was found to exhibit on...Research on nickel-based superconductors has progressed from infinite-layer LaNiO_(2) to finite-layer La_(6)Ni_(5)O_(12),and most recently to the Ruddlesden-Popper phase La_(3)Ni_(2)O_(7),which was found to exhibit onset of superconductivity at∼80K under a pressure of∼16 GPa.Using density functional calculations and multi-orbital,multi-atom cluster exact diagonalization that includes local exchange and Coulomb interactions,here we analyze the pressure dependent low-energy electronic states of the Ni_(2)O_(9) cluster,relevant for the bilayer phase of La_(3)Ni_(2)O_(7).We quantify the various possible spin states and the exchange and superexchange mechanisms of the Ni_(2)O_(9) cluster are quantified through the involvement of the Ni-3d_(3z^(2)−r^(2)) orbitals and the atomic Hund’s rule exchange,the apical bridging O-2pz orbitals,and the orbitals involved in the formation of local Zhang-Rice singlet like states.We find that the leading configurations contributing to the cluster ground-states both for nominal valence and also with local charge fluctuations,do not involve occupation of the apical oxygen;instead,they favor the formation of in-plane Zhang-Rice singlet-like states between an O ligand hole and the Ni 3d_(z^(2)−y^(2)) orbital.We also highlight two possible charge and spin ordered states suggested by our cluster results,that are nearly degenerate at all relevant pressures within our modeling.展开更多
By using density matrix renormalization group （DMRG） method a model for organic molecule-based ferromagnetic chain is proposed. It is found that the ground states of Undoped and doped systems both exhibit ferrimagne...By using density matrix renormalization group （DMRG） method a model for organic molecule-based ferromagnetic chain is proposed. It is found that the ground states of Undoped and doped systems both exhibit ferrimagnetic ordering. The e-e repulsion plays an important role in the stability of the ferromagnetic state either in doped system or undoped system. For the undoped system, each unit cell coatains half of the total spins, which is consistent with Lieb＇s theorem. It is convinced that when the system is doped with one electron, a charge density wave is excited, which decreases the amplitude of spin density wave,therefore acting against the stability of ferromagnetic state.展开更多
Compound 1 was first synthesized and characterized. Its crystal structure and magnetic property were determined and investigated. Discussion about the molecule packing in crystal and the macroscopic magnetism was also...Compound 1 was first synthesized and characterized. Its crystal structure and magnetic property were determined and investigated. Discussion about the molecule packing in crystal and the macroscopic magnetism was also presented, in combination with computing study of the spatial distribution over the molecule.展开更多
Gamma-ray (GRBs) and X-ray Bursts are millisecond-10 and 1000 seconds-long events of unknown origin. Recent simulations of the merger of binary neutron star systems do not generate a magnetically dominated c...Gamma-ray (GRBs) and X-ray Bursts are millisecond-10 and 1000 seconds-long events of unknown origin. Recent simulations of the merger of binary neutron star systems do not generate a magnetically dominated called funnel nor a relativistic outflow. New models for the detection the afterglow of GRB 121024A, measured 0.15 days after the burst, invoke anisotropy as required to produce the complex microphysics of realistic shocks in relativistic jets. On the other hand the non-thermal gamma-rays are supposed to be produced by a fireball of relativistic e<sup>?</sup>e<sup>+</sup> pairs that are created by annihilation of neutrino-antineutrino pairs in the vicinity of the hot, merged object. It is also known that in a system of a large number of fermions with pairs, gravitational interaction occurs a spontaneous breaking of the vacuum spatial symmetry, accompanied by gravitational mass defect. If spherical symmetry is broken, as in the known case of the merger scenario where a rapidly rotating disk can be formed and material is pulled away from rotation axis by centrifugal forces, then a baryon-free funnel along the rotation axes may allow relativistic beam of γ’s and e<sup>?</sup>e<sup>+</sup> to escape. It might lead to matter ejection with Lorentz factors of ~10<sup>2</sup> - 103</sup> which are in the right range to enable copious gamma production during shock interaction with ambient interstellar gas. Here we show that the space rays generation mechanism on a method of direct transformation of intergalactic gamma-rays to the proton current on spin shock-waves ensure precise agreement between generated proton currents (spin shock waves theory) with the angular distribution data of Galactic gamma-rays as well as for the individual pulses of gamma-/X-ray bursts. There is a precise confirmation of the generated currents (theory) with the burst radiation data characterized by the standard deviation of ±1% in intensity in relative units within the sensitivity of the equipment. Thus, it was found that the spin angular momentum conservation law (equation of dynamics of spin shock waves) in the X-ray/gamma ranges is fulfilled exactly in real time. The next step involves setting the inverse problem of determining the wave function disturbance on the differential of measured smoothing pulses. In the asymptotic large times the problem is reduced to the solutions of the functional equation with shift of the argument. This will give additional information about the change speed of the wave, as well as on the interaction.展开更多
Heteroatom-doped carbon has been demonstrated to be one of the most promising non-noble metal catalysts with high catalytic activity and stability through the modification of the electronic and geometric structures.In...Heteroatom-doped carbon has been demonstrated to be one of the most promising non-noble metal catalysts with high catalytic activity and stability through the modification of the electronic and geometric structures.In this study,we develop a novel solvent method to prepare interconnected N,S co-doped three-dimensional（3D）carbon networks with tunable nanopores derived from an asso-ciated complex based on melamine and sodium dodecylbenzene sulfonate（SDBS）.After the intro-duction of silica templates and calcination,the catalyst exhibits 3D networks with interconnected 50-nm pores and partial graphitization.With the increase of the number of Lewis base sites caused by the N doping and change of the carbon charge and spin densities caused by the S doping,the designed N,S co-doped catalyst exhibits a similar electrochemical activity to that of the commercial 20-wt%Pt/C as an oxygen reduction reaction catalyst.In addition,in an aluminum-air battery,the proposed catalyst even outperforms the commercial 5-wt%Pt/C catalyst.Both interconnected porous structures and synergistic effects of N and S contribute to the superior catalytic perfor-mance.This study paves the way for the synthesis of various other N-doped and co-doped carbon materials as efficient catalysts in electrochemical energy applications.展开更多
Comprehensive Summary A design strategy towards stable fluorenyl radicals(FRs)has been developed through introducing donor-π-radical(D-π-R)conjugation,facilitated by the linkage of amine N atoms and FR centers via p...Comprehensive Summary A design strategy towards stable fluorenyl radicals(FRs)has been developed through introducing donor-π-radical(D-π-R)conjugation,facilitated by the linkage of amine N atoms and FR centers via phenyl or 9-anthryl moieties.Four FRs,with or without N atom containing protecting groups,were designed and synthesized for comparative analysis.展开更多
In this paper,a formalism is presented for the helicity amplitude analysis of the decays Ψ(2S)→γ_(1)χ_(c)J,χ_(c)J→γ_(2)V(V=p^(0),φ,ω)(subscripts 1 and 2 are used to distinguish the two radiative photons),and ...In this paper,a formalism is presented for the helicity amplitude analysis of the decays Ψ(2S)→γ_(1)χ_(c)J,χ_(c)J→γ_(2)V(V=p^(0),φ,ω)(subscripts 1 and 2 are used to distinguish the two radiative photons),and the polarization expressions of the P-wave charmonia χ_(c)J and the vector mesons p^(0),φ,ω for experimental measurements at an electron-positron collider.In addition,we derive formulae for the angular distributions of χ_(c1,2)→γV to extract the degree of transverse polarization P_(T) of e^(+)e^(-)pairs with symmetric beam energy as well as the ratios of two helicity amplitudes x(in χ_(c1) decays)and x,y(in χ_(c2) decays),which represent the relative magnitudes of transverse to longitudinal polarization amplitude.The results are validated by Monte Carlo simulation.Finally,the statistical sensitivity of P_(T),x,and y are estimated based on the large Ψ(2S)data samples collected at current and proposed future e^(+)e^(-)colliderexperiments.展开更多
Fe-based superconductors represent a fascinating class of materials,extensively studied for their complex interplay of superconductivity,magnetism,spin density waves,and nematicity,along with the interactions among th...Fe-based superconductors represent a fascinating class of materials,extensively studied for their complex interplay of superconductivity,magnetism,spin density waves,and nematicity,along with the interactions among these orders.An intriguing yet unexplained phenomenon observed in Fe-based superconductors is the emergence of superconductivity below 25K in the non-superconducting parent compound SrFe_(2)As_(2)following exposure to water at its surface.In this study,we employed in situ angle-resolved photoemission spectroscopy and low-energy electron diffraction to meticulously examine the electronic structure evolution of SrFe_(2)As_(2)upon in situ water dosing.Our findings indicate that water dosing markedly attenuates the spin density wave phase and surface Sr reconstruction while preserving the nematic order in SrFe_(2)As_(2).Furthermore,we detected an enhancement in the spectral weight of bands near the Fermi level.Our observations highlight the critical role of the intricate interplay among various orders induced by water dosing,which effectively modifies the band structure and favors the emergence of superconductivity in SrFe_(2)As_(2).展开更多
基金the full support of the National Natural Science Foundation of China(62071154,51272052 and50902040)the Natural Science Foundation of Heilongjiang Province of China(LH2020B011 and LH2019B006)the Scientific Research Projects of Basic Scientific Research Operational Expenses of Heilongjiang Provincial Colleges and Universities(2021-KYYWF-0171)。
文摘The integration of machine learning and electrocatalysis presents nota ble advancements in designing and predicting the performance of chiral materials for hydrogen evolution reactions(HER).This study utilizes theoretical calculations and machine learning techniques to assess the HER performance of both chiral and achiral M-N-SWCNTs(M=In,Bi,and Sb)single-atom catalysts(SACs).The stability preferences of metal atoms are dependent on chirality when interacting with chiral SWCNTs.The HER activity of the right-handed In-N-SWCNT is 5.71 times greater than its achiral counterpart,whereas the left-handed In-N-SWCNT exhibits a 5.12-fold enhancement.The calculated hydrogen adsorption free energy for the right-handed In-N-SWCNT reaches as low as-0.02 eV.This enhancement is attributed to the symmetry breaking in spin density distribution,transitioning from C_(2V)in achiral SACs to C_(2)in chiral SACs,which facilitates active site transfer and enhances local spin density.Right-handed M-N-SWCNTs exhibit superiorα-electron separation and transport efficiency relative to left-handed variants,owing to the chiral induced spin selectivity(CISS)effect,with spin-upα-electron density reaching 3.43×10^(-3)e/Bohr^(3)at active sites.Machine learning provides deeper insights,revealing that the interplay of weak spatial electronic effects and appropriate curvature-chirality effects significantly enhances HER performance.A weaker spatial electronic effect correlates with higher HER activity,larger exchange current density,and higher turnover frequency.The curvature-chirality effect undersco res the influence of intrinsic structures on HER performance.These findings offer critical insights into the role of chirality in electrocatalysis and propose innovative approaches for optimizing HER through chirality.
文摘Elastic neutron diffraction measurements were performed on single crystals to study the ground state below the mysterious exotic transition temperature 0.86 K. An antiferromagnetic order with a tiny moment of 0.027 μB per formula is formed as the ground state for CeOs4Sb12 below the transition point. Our neutron data gives the evidence of spin density wave state for CeOs4Sb12 in this work.
基金Supported by the National Natural Science Foundation of China(No.21061009)
文摘A supramolecular 1D ferromagnetic system was studied experimentally as well as theoretically.Hybrid density functional theory（DFT） calculations were based on the X-ray analysis.The results of DFT calculations and McConnell mechanism have contributed to the understanding of the factors governing the exchange coupling of magnetism in the crystal packing.Both the experimental evidence and theoretical calculation indicate that spin density in 2-iodo nitronyl nitroxide（INN） radicals confirms 1D ferromagnetic chain with inter-chain antiferromagnetic interaction.
基金supported by the National Key Research and Development Projects of China(Grant Nos.2023YFA1406103,2024YFA1611302,2024YFA1409200,and 2022YFA1403402)the National Natural Science Foundation of China(Grant Nos.12374142,12304170,12025408,12404179,and U23A6003)+2 种基金Beijing National Laboratory for Condensed Matter Physics(Grant No.2024BNLCMPKF005)the Chinese Academy of Sciences President’s International Fellowship Initiative(Grant No.2024PG0003)supported by the Synergetic Extreme Condition User Facility(SECUF,https://cstr.cn/31123.02.SECUF)。
文摘The recent discovery of superconductivity in La_(3)Ni_(2)O_(7-δ)with a transition temperature Tc close to 80 K at high pressures has attracted significant attention,due particularly to a possible density wave(DW)transition occurring near the superconducting dome.Identifying the type of DW order is crucial for understanding the origin of superconductivity in this system.However,owing to the presence of La4Ni3O10 and other intergrowth phases in La_(3)Ni_(2)O_(7-δ)samples,extracting the intrinsic information from the La_(3)Ni_(2)O_(7) phase is challenging.In this study,we employed ^(139)La nuclear quadrupole resonance(NQR)measurements to eliminate the influence of other structural phases in the sample and obtain microscopic insights into the DW transition in La_(3)Ni_(2)O_(7-δ).Below the DW transition temperature T_(DW)∼153 K,we observe a distinct splitting in the±5/2↔±7/2 transition of the NQR resonance peak at the La(2)site,while only a line broadening is seen in the±3/2↔±5/2 transition peak.Through further analysis of the spectra,we show that the line splitting is due to a unidirectional charge modulation.A magnetic line broadening is also observed below T_(DW),accompanied by a large enhancement of the spin-lattice relaxation rate,indicating the formation of magnetically ordered moments in the DW state.Our results suggest a simultaneous formation of charge-and spin-density wave orders in La_(3)Ni_(2)O_(7-δ),thereby offering critical insights into the electronic correlations in Ni-based superconductors.
基金supported by the National Natural Science Foundation of China(NSFC)(No.11974281)the Natural Science Basic Research Plan in Shaanxi Province of China(No.2020JM-116)。
文摘The evolution of the spin density vectors(SDVs) is studied in a strongly focused composite field. It is found that the SDVs can be spiral along the propagation axis, and they are perpendicular to the ysdirection on the ysaxis. This behavior is governed by the Gouy phase difference between the field polarization components. The 60° rotation of the spatial distribution of the transverse SDVs is also generated, which is found to be controlled by the Gouy phase difference between the field orbital angular momentum modes. Additionally, the spin density singularities are observed in the evolution of the SDVs.
基金Project supported by the National Basic Research Program of China （No. 2006CB601102）, the National Natural Science Foundation of China （Nos 20503001, 20490210, NSFC/RGC 20318001）, the Doctoral Program Foundation of Education Minister （No. 20030001066）.
文摘In order to shed light upon the nature and mechanism of 4f-3d magnetic exchange interactions, a series of binuclear complexes of lanthanide（3＋） and chromium（3＋） with the general formula [Ln（L）5（H2O）2Cr（CN）6]·mL· nH2O （Ln=La （1）, Ce （2）, Pr （3）, Nd （4）; x=5, y=2, m=1 or 2, n=2 or 2.5; L=2-pyrrolidinone） and [Ln（L）4（H2O）3Cr（CN）6] ·nH2O （Ln=Sm （5）, Eu （6）, Gd （7）, Tb （8）, Dy （9）, Er （10）; x=4, y=3, m=0, n= 1.5 or 2.0; L=2-pyrrolidinone） were prepared and the X-ray crystal structures of complexes 2, 6 and 7 were determined. All the compounds consist of a Ln-CN-Cr unit, in which Ln^3＋ in a square antiprism environment is bridged to an octahedral coordinated Cr^3＋ ion through a cyano group. The magnetic properties of the complexes 3 and 6-10 show an overall antiferromagnetic behavior. The fitting to the experimental magnetic susceptibilities of 7 give g= 1.98, J=0.40 cm^-1, zJ＇= -0.21 cm^-1 on the basis of a binuclear spin system （Scd=7/2, Scr=3/2）, revealing an intra-molecular Gd^3＋-Cr^3＋ ferromagnetic interaction and an inter-molecular antiferromagnetic interaction. For 7 the calculation of quantum chemical density functional theory （DFT）, combined with the broken symmetry approach, showed that the calculated spin coupling constant was 20.3 cm^-1, supporting the observation of weak ferromagnetic intra-molecular interaction in 7. The spin density distributions of 7 in both the high spin ground state and the broken symmetry state were obtained, and the spin coupling mechanism between Gd^3＋ and Cr^3＋ was discussed.
基金Supported by the National Natural Science Foundation of China(12247121)。
文摘We investigate the spin density matrix of Ω− in the Cartesian coordinate system of baryon-antibaryon pairs produced in e+e−annihilation.Using the helicity formalism of Jacob and Wick,we derive the expression for the spin-3/2 density matrices.Our analysis is based on the angular distribution of the process e+e−→ψ(3686)→Ω−Ω¯^(+ )in the BESIII experiment.By decomposing the polarization state of Ω− particles along different coordinate axes,we examine the polarization dependence of the cross-section.Our results demonstrate that Ω− particles exhibit varying degrees of tensor polarization along the x-,y-,and z-axes,as well as weak vector polarization and rank-3 tensor polarization along the y-axis.To the best of our knowledge,this is the first study to calculate the polarization dependence of the cross-section distributions for the annihilation process e+e−→Ω−Ω¯^(+).Our theoretical predictions are in good agreement with the experimental measurements.
基金support from the National Natural Science Foundation of China(523B2061)National Innovative Talents Program(GG2090007001)University of Science and Technology of China Startup Program(KY2090000044).
文摘Recently,a signature of high-temperature superconductivity above the liquid nitrogen temperature(77 K)was reported for La_(3)Ni_(2)O_(7−δ) under pressure.This finding immediately stimulated intense interest in the possible mechanism of high-Tc superconductivity in double-layer nickelates.Notably,the pressure-dependent phase diagram inferred from transport measurements indicates that the superconductivity under high pressure emerges from the suppression of density-wave-like order at ambient pressure,which is similar to high-temperature superconductors.Therefore,clarifying the exact nature of the density-wave-like transition is important for determining the superconducting mechanism in double-layer nickelates.Here,nuclear magnetic resonance(NMR)spectroscopy of 139La nuclei was performed to study the density-wave-like transition in a single crystal of La_(3)Ni_(2)O_(7−δ.)At high temperatures,two sets of sharp 139La NMR peaks are clearly distinguishable from a broad background signals,which are ascribed to La(1)sites from two bilayer Ruddlesden-Popper phases with different oxygen vacancyδ.As the temperature decreases,the temperature-dependent^(139)La NMR spectra and nuclear spin-lattice relaxation rate(1/T_(1))for both La(1)sites provide evidence of spin-density-wave(SDW)ordering below the transition temperature(T_(SDW)),which is approximately 150 K.The anisotropic splitting in the NMR spectra suggests the formation of a possible double spin stripe with magnetic moments aligned along the c-axis.Furthermore,we studied the pressure-dependent SDW transition up to∼2.7 GPa.Surprisingly,the TSDW inferred from NMR measurements of both La(1)sites increases with increasing pressure,which is opposite to the results from previous transport measurements under pressure and suggests an intriguing phase diagram between superconductivity and SDW.In contrast,the present^(139)La NMR is insensitive to the possible charge-density-wave(CDW)order in the Ni-O planes.All these results will be helpful for building a connection between superconductivity and magnetic interactions in double-layer nickelates.
基金the financial support from National Natural Science Foundation of China(22363001,22378379,22479032,22022814)the National Key R&D Project(2022YFA1503900)+6 种基金the Natural Science Special Foundation of Guizhou University(No.202140)National Natural Science Foundation of China for Single-Atom Catalysis(22388102)the Youth Innovation Promotion Association CAS(Y2021057)Dalian Science Foundation for Distinguished Young Scholars(2021RJ10)Grant.YLU-DNL Fund(2022010)the Young Top-notch Talents of Liaoning Province(XLYC2203140)the Liaoning Foundation for Distinguished Young Scholars(2025JH6/101100011).
文摘UiO-66-H MOFs can effectively catalyze the direct selective oxidation of methane(DSOM)to high value-added oxygenates under mild conditions.However,UiO-66-NH_(2)with benzene-1,4-dicarboxylate(NH_(2)-BDC)ligand modifying the Zr-oxo nodes exhibits relatively inferior catalytic performance for DSOM.Here,a combination of density functional theory(DFT)calculations and experiments was employed to explore the underlying reasons for the limited catalytic activity of UiO-66-NH_(2).The results indicate that the methane hydroxylation performance of UiO-66-NH_(2)is almost unaffected by the increase of·OH concentration.This is attributed to the formation of substantial non-covalent hydrogen bonds between the oxygen atoms of oxygenic species on the Zr-oxo nodes and the hydrogen atoms of-NH_(2)groups,which diminishes the spin density distribution on the active sites of(·OH)m/UiO-66-NH_(2),leading to minimal change of the adsorption energy of CH_(4).Additionally,the calculated adsorption energies(Eads)of CH_(4)exhibit a linear relationship with the catalytic activity of UiO-66-NH_(2)for DSOM reaction.
基金Project supported by the National Natural Science Foundation of China(Grant No.11674392)the Ministry of Science and Technology of China,National Program on Key Research Project(Grant No.2016YFA0300504)the Research Funds of Remnin University of China(Grant No.18XNLG24).
文摘In quasi-one-dimensional(q1D) quantum antiferromagnets, the complicated interplay of intrachain and interchain exchange couplings may give rise to rich phenomena. Motivated by recent progress on field-induced phase transitions in the q1D antiferromagnetic(AFM) compound YbAlO3, we study the phase diagram of spin-1/2 Heisenberg chains with Ising anisotropic interchain couplings under a longitudinal magnetic field via large-scale quantum Monte Carlo simulations,and investigate the role of the spin anisotropy of the interchain coupling on the ground state of the system. We find that the Ising anisotropy of the interchain coupling can significantly enhance the longitudinal spin correlations and drive the system to an incommensurate AFM phase at intermediate magnetic fields, which is understood as a longitudinal spin density wave(LSDW). With increasing field, the ground state changes to a canted AFM order with transverse spin correlations. We further provide a global phase diagram showing how the competition between the LSDW and the canted AFM states is tuned by the Ising anisotropy of the interchain coupling.
基金Project supported by the National Basic Research Program of China(Grants No.2011CB921602)the National Natural Science Foundation of China(Grants No.20121318158)
文摘The spin transport properties of S–Au–S junction and Au–Au–Au junction between Au nanowires are investigated with density functional theory and the non-equilibrium Green＇s function. We mainly focus on the spin resonance transport properties of the center Au atom. The breaking of chemical bonds between anchor atoms and center Au atom significantly influences their spin transmission characteristics. We find the 0.8 eV orbital energy shift between anchor S atoms and the center Au atom can well protect the spin state stored in the S–Au–S junction and efficiently extract its spin state to the current by spin resonance mechanism, while the spin interaction of itinerant electrons and the valence electron of the center Au atom in the Au–Au–Au junction can extract the current spin information into the center Au atom. Fermi energy drift and bias-dependent spin filtering properties of the Au–Au–Au junction may transform information between distance, bias,and electron spin. Those unique properties make them potential candidates for a logical nanocircuit.
基金supported by National Natural Science Foundation of China(Nos.51772213,12004283,12274324)Science and Technology Commission of Shanghai Municipality(No 21JC405700)Shanghai Key Laboratory of Special Artificial Microstructure Materials and Technology.
文摘Development of a high-performance bifunctional catalyst is essential for the actual implementation of zinc-air batteries in practical applications.Herein,a bifunctional cathode of Co_(3)S_(4)/FeS heterogeneous nanoparticles embedded in Co/Fe single-atom-loaded nitrogen-doped carbon nanosheets is designed.Cobalt-iron sulfides and single atomic sites with Co-N_(4)/Fe-N_(4)configurations are confirmed to coexist on the carbon matrix by EXAFS spectroscopy.3D self-supported super-hydrophobic multiphase composite cathode provides abundant active sites and facilitates gas–liquid-solid three-phase interface reactions,resulting in excellent electrocatalytic activity and batteries performance,i.e.,an OER overpotential(η_(10))of 260 mV,a half-wave potential(E_(1/2))of 0.872 V for ORR,aΔE of 0.618 V,and a discharge power density of 170 mW cm^(−2),a specific capacity of 816.3 mAh g^(−1).DFT analysis shows multiphase coupling of sulfide heterojunction through single-atomic metal doped carbon nanosheets reduces offset on center of electronic density of states before and after oxygen adsorption,and spin density of adsorbed oxygen with same spin orientation,leading to weakened charge/spin interactions between adsorbed oxygen and substrate,and a lowered oxygen adsorption energy to accelerate OER/ORR.
基金the support of the National Natural Science Foundation of China(Grant No.12174278)support from the National Natural Science Foundation of China(Grant No.12422407)+3 种基金the Startup Funding from Soochow Universitythe Priority Academic Program Development of Jiangsu Higher Education Institutionssupported by the Quantum Matter Institute(QMI)at the University of British Columbiathe Natural Sciences and Engineering Research Council of Canada(NSERC).
文摘Research on nickel-based superconductors has progressed from infinite-layer LaNiO_(2) to finite-layer La_(6)Ni_(5)O_(12),and most recently to the Ruddlesden-Popper phase La_(3)Ni_(2)O_(7),which was found to exhibit onset of superconductivity at∼80K under a pressure of∼16 GPa.Using density functional calculations and multi-orbital,multi-atom cluster exact diagonalization that includes local exchange and Coulomb interactions,here we analyze the pressure dependent low-energy electronic states of the Ni_(2)O_(9) cluster,relevant for the bilayer phase of La_(3)Ni_(2)O_(7).We quantify the various possible spin states and the exchange and superexchange mechanisms of the Ni_(2)O_(9) cluster are quantified through the involvement of the Ni-3d_(3z^(2)−r^(2)) orbitals and the atomic Hund’s rule exchange,the apical bridging O-2pz orbitals,and the orbitals involved in the formation of local Zhang-Rice singlet like states.We find that the leading configurations contributing to the cluster ground-states both for nominal valence and also with local charge fluctuations,do not involve occupation of the apical oxygen;instead,they favor the formation of in-plane Zhang-Rice singlet-like states between an O ligand hole and the Ni 3d_(z^(2)−y^(2)) orbital.We also highlight two possible charge and spin ordered states suggested by our cluster results,that are nearly degenerate at all relevant pressures within our modeling.
基金the National Natural Science Foundation of China under
文摘By using density matrix renormalization group （DMRG） method a model for organic molecule-based ferromagnetic chain is proposed. It is found that the ground states of Undoped and doped systems both exhibit ferrimagnetic ordering. The e-e repulsion plays an important role in the stability of the ferromagnetic state either in doped system or undoped system. For the undoped system, each unit cell coatains half of the total spins, which is consistent with Lieb＇s theorem. It is convinced that when the system is doped with one electron, a charge density wave is excited, which decreases the amplitude of spin density wave,therefore acting against the stability of ferromagnetic state.
文摘Compound 1 was first synthesized and characterized. Its crystal structure and magnetic property were determined and investigated. Discussion about the molecule packing in crystal and the macroscopic magnetism was also presented, in combination with computing study of the spatial distribution over the molecule.
文摘Gamma-ray (GRBs) and X-ray Bursts are millisecond-10 and 1000 seconds-long events of unknown origin. Recent simulations of the merger of binary neutron star systems do not generate a magnetically dominated called funnel nor a relativistic outflow. New models for the detection the afterglow of GRB 121024A, measured 0.15 days after the burst, invoke anisotropy as required to produce the complex microphysics of realistic shocks in relativistic jets. On the other hand the non-thermal gamma-rays are supposed to be produced by a fireball of relativistic e<sup>?</sup>e<sup>+</sup> pairs that are created by annihilation of neutrino-antineutrino pairs in the vicinity of the hot, merged object. It is also known that in a system of a large number of fermions with pairs, gravitational interaction occurs a spontaneous breaking of the vacuum spatial symmetry, accompanied by gravitational mass defect. If spherical symmetry is broken, as in the known case of the merger scenario where a rapidly rotating disk can be formed and material is pulled away from rotation axis by centrifugal forces, then a baryon-free funnel along the rotation axes may allow relativistic beam of γ’s and e<sup>?</sup>e<sup>+</sup> to escape. It might lead to matter ejection with Lorentz factors of ~10<sup>2</sup> - 103</sup> which are in the right range to enable copious gamma production during shock interaction with ambient interstellar gas. Here we show that the space rays generation mechanism on a method of direct transformation of intergalactic gamma-rays to the proton current on spin shock-waves ensure precise agreement between generated proton currents (spin shock waves theory) with the angular distribution data of Galactic gamma-rays as well as for the individual pulses of gamma-/X-ray bursts. There is a precise confirmation of the generated currents (theory) with the burst radiation data characterized by the standard deviation of ±1% in intensity in relative units within the sensitivity of the equipment. Thus, it was found that the spin angular momentum conservation law (equation of dynamics of spin shock waves) in the X-ray/gamma ranges is fulfilled exactly in real time. The next step involves setting the inverse problem of determining the wave function disturbance on the differential of measured smoothing pulses. In the asymptotic large times the problem is reduced to the solutions of the functional equation with shift of the argument. This will give additional information about the change speed of the wave, as well as on the interaction.
基金supported by the National Natural Science Foundation of China (51674297)the Natural Science Foundation of Hunan Province (2016JJ2137)the Fundamental Research Funds for the Central Universities of Central South University (2015cx001)~~
文摘Heteroatom-doped carbon has been demonstrated to be one of the most promising non-noble metal catalysts with high catalytic activity and stability through the modification of the electronic and geometric structures.In this study,we develop a novel solvent method to prepare interconnected N,S co-doped three-dimensional（3D）carbon networks with tunable nanopores derived from an asso-ciated complex based on melamine and sodium dodecylbenzene sulfonate（SDBS）.After the intro-duction of silica templates and calcination,the catalyst exhibits 3D networks with interconnected 50-nm pores and partial graphitization.With the increase of the number of Lewis base sites caused by the N doping and change of the carbon charge and spin densities caused by the S doping,the designed N,S co-doped catalyst exhibits a similar electrochemical activity to that of the commercial 20-wt%Pt/C as an oxygen reduction reaction catalyst.In addition,in an aluminum-air battery,the proposed catalyst even outperforms the commercial 5-wt%Pt/C catalyst.Both interconnected porous structures and synergistic effects of N and S contribute to the superior catalytic perfor-mance.This study paves the way for the synthesis of various other N-doped and co-doped carbon materials as efficient catalysts in electrochemical energy applications.
基金supported by Natural Science Foundation of China(22175128)starting grants of Tianjin University.
文摘Comprehensive Summary A design strategy towards stable fluorenyl radicals(FRs)has been developed through introducing donor-π-radical(D-π-R)conjugation,facilitated by the linkage of amine N atoms and FR centers via phenyl or 9-anthryl moieties.Four FRs,with or without N atom containing protecting groups,were designed and synthesized for comparative analysis.
基金Supported by the National Natural Science Foundation of China(11805064,11975118)State Key Laboratory of Nuclear Physics and Technology,Peking university(NPT2025KFY03)。
文摘In this paper,a formalism is presented for the helicity amplitude analysis of the decays Ψ(2S)→γ_(1)χ_(c)J,χ_(c)J→γ_(2)V(V=p^(0),φ,ω)(subscripts 1 and 2 are used to distinguish the two radiative photons),and the polarization expressions of the P-wave charmonia χ_(c)J and the vector mesons p^(0),φ,ω for experimental measurements at an electron-positron collider.In addition,we derive formulae for the angular distributions of χ_(c1,2)→γV to extract the degree of transverse polarization P_(T) of e^(+)e^(-)pairs with symmetric beam energy as well as the ratios of two helicity amplitudes x(in χ_(c1) decays)and x,y(in χ_(c2) decays),which represent the relative magnitudes of transverse to longitudinal polarization amplitude.The results are validated by Monte Carlo simulation.Finally,the statistical sensitivity of P_(T),x,and y are estimated based on the large Ψ(2S)data samples collected at current and proposed future e^(+)e^(-)colliderexperiments.
基金supported by the National Nature Science Foundation of China[Grant Nos.92365204 and 12274298(Z.K.Liu)]the National Key R&D program of China[Grant No.2022YFA1604400/03(Z.K.Liu)]Zhangjiang Laboratory(Y.M.Zhang).The authors thank BL02B at the Shanghai Synchrotron Radiation Facility supported by the National Natural Science Foundation of China(Contract No.11227902).
文摘Fe-based superconductors represent a fascinating class of materials,extensively studied for their complex interplay of superconductivity,magnetism,spin density waves,and nematicity,along with the interactions among these orders.An intriguing yet unexplained phenomenon observed in Fe-based superconductors is the emergence of superconductivity below 25K in the non-superconducting parent compound SrFe_(2)As_(2)following exposure to water at its surface.In this study,we employed in situ angle-resolved photoemission spectroscopy and low-energy electron diffraction to meticulously examine the electronic structure evolution of SrFe_(2)As_(2)upon in situ water dosing.Our findings indicate that water dosing markedly attenuates the spin density wave phase and surface Sr reconstruction while preserving the nematic order in SrFe_(2)As_(2).Furthermore,we detected an enhancement in the spectral weight of bands near the Fermi level.Our observations highlight the critical role of the intricate interplay among various orders induced by water dosing,which effectively modifies the band structure and favors the emergence of superconductivity in SrFe_(2)As_(2).
