Evidence of spin density wave of CeOs_4Sb_(12)

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.

1D Ferromagnetic Interaction of 2-Iodo Nitronyl Nitroxide Radical Confirmed by Spin Density Calculation

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.

Evolution of spin density vectors in a strongly focused composite field

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.

Cyano-bridged Ln^3＋-Cr^3＋ Binuclear Complexes [Ln（L）x（H2O）y^- Cr（CN）6]·mL·nH2O （Ln=La-Nd, x=5, y=2, m=1 or 2, n=2 or 2.5; Ln-Sm-Dy, Er, x=4, y=3, m=0, n=1.5 or 2.0; L= 2-pyrrolidinone）： Structure, Magnetism and Spin Density Map

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.

Spin density matrix forΩ−and its polarization alignment in ψ(3686)→Ω−Ω¯^(+)

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.

Role of the spin anisotropy of the interchain interaction in weakly coupled antiferromagnetic Heisenberg chains

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.

Spin resonance transport properties of a single Au atom in S–Au–S junction and Au–Au–Au junction

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.

Superhydrophobic Co/Fe sulfide nanoparticles and single-atoms doped carbon nanosheets composite air cathode for high-performance zinc-air batteries

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.

DMRG Studies on Properties of Undoped and Doped Molecule-Based Ferromagnetic Chain

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.

Crystal Structure and Magnetic Studies of a New Nitronyl Nitroxide Compound

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.

On the Gamma-Ray Bursts Origin

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?e+ 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?e+ to escape. It might lead to matter ejection with Lorentz factors of ~102 - 103 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.

Self-assembled three-dimensional carbon networks with accessorial Lewis base sites and variational electron characteristics as efficient oxygen reduction reaction catalysts for alkaline metal-air batteries

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.

Reactivity,Regioselectivity,and Synthetic Application of 2-Pyrenyl Units in Scholl Reactions

We herein report the reactivity and regioselectivity of 2-pyrenyl as a coupling unit in Scholl reactions.On the basis of the Scholl reactions of hexaarylbenzene substrates,we have found that pyrenyl units are preferably oxidized over naphthyl and phenyl units under appropriate Scholl reaction conditions,allowing divergent synthesis through a highly controllable intramolecular coupling sequence.We find that the C1 and C3 positions of the 2-pyrenyl unit are the favorable sites for intramolecular coupling while C4 is not reactive to allow further coupling.The reactivity and regioselectivity pattern can be explained by the spin density distribution,which shows that carbon-carbon bonds preferably form at sites with higher positive spin density.Guided by these findings,we successfully synthesized a double helicene and a sextuple helicene through the controlled Scholl reactions of 2-pyrenyl units.

Successive Free-Radical C(sp^(2))-C(sp^(2)) Coupling Reactions to Form Graphene

Graphene is of great interest because of its exciting properties and potential applications,but its production on a large-scale still presents considerable challenges.Herein,we report the synthesis of predominately few-layer graphene,due toπ–πstacking,and single-layer graphene from reaction between hexabromobenzene and Na metal,followed by annealing to improve crystallinity.The reaction proceeds via a free-radical C(sp^(2))–C(sp^(2))coupling mechanism,which is supported by theoretical calculations.The graphene can host unpaired spin electrons,leading to a short acquisition time for a solidstate nuclear magnetic resonance 13C spectrum from unlabeled graphene,which is ascribed to the very short spin-lattice relaxation time.High catalytic activity for transforming amine to imine with a conversion of>99%and a yield of∼97%is demonstrated,and high electronic conductivity of∼105 S·m^(−1) is found by terahertz spectroscopy.The reaction delivers a method for synthesizing graphene with a high spin concentration from perbrominated benzene molecules by using an active metallic agent,such as Na,Li,or Mg.

Study of parity violation inΛ^(+)_(c)→ΦρandΛ^(+)_(c)→ωρdecays

CP violation in baryonic decays has not been significantly observed.With large data events accumulated at e+e-colliders or the Large Hadron Collider,charmed baryon decays would provide a promising laboratory to test CP symmetry.In this study,we formulateΛ^(+)_(c)→ΦρandΛ^(+)_(c)→ωρdecays for the measurement of their asymmetry parameters in weak decays at the BESII or LHCb experiments.The polarization transfer is analyzed in the two processes of e+e-→Λ^(+)_(c)Λ^(-)_(c)andΛ^(o)_(b)→Λ^(+)_(c)π^(-),and the formulas for the joint angular distribution of these processes are provided.The sensitivity of the measurement of the asymmetry parameters of the above two decay processes is estimated for future experiments.

Phenomenological study of J/ψ→Ξ^(0)(Λπ^(0))ˉΞ^(0)(Λγ)decays

The measurement of decay parameters is one of the important goals of particle physics experiments,and the measurement serves as a probe to search for evidence of CP violation in baryonic decays.The experimental results will aid in advancing existing theoretical research and establishing new experimental objectives.In this study,we formulate the asymmetric parameters that characterize parity violation,and then derive formulas for the measurement of CP violation.The formulae for the joint angular distribution of the full decay chain as well as the polarization observable of Ξ^(0),Ξ¯^(0),Λ,and Λ¯are also provided for experiments.Lastly,we evaluated the sensitivity of two asymmetric parameters:αΞ0→Λπ0(abbreviated asαΞ0)andαΞ¯0→Λ¯γ(abbreviated asαΞ¯0)for future experimental measurements.

Computational studies of σ-type weak interactions between NCO/NCS radicals and XY(X = H,Cl;Y = F,Cl,and Br)

The triatomic radicals NCO and NCS are of interest in atmospheric chemistry,and both the ends of these radicals can potentially serve as electron donors during the formation of σ-type hydrogen/halogen bonds with electron acceptors XY(X = H,Cl;Y = F,Cl,and Br).The geometries of the weakly bonded systems NCO/NCS···XY were determined at the MP2/aug-cc-pVDZ level of calculation.The results obtained indicate that the geometries in which the hydrogen/halogen atom is bonded at the N atom are more stable than those where it is bonded at the O/S atom,and that it is the molecular electrostatic potential(MEP)-not the electronegativity-that determines the stability of the hydrogen/halogen bond.For the same electron donor(N or O/S) in the triatomic radical and the same X atom in XY,the bond strength decreases in the order Y = F > Cl > Br.In the hydrogen/halogen bond formation process for all of the complexes studied in this work,transfer of spin electron density from the electron donor to the electron acceptor is negligible,but spin density rearranges within the triatomic radicals,being transferred to the terminal atom not interacting with XY.

Theoretical Studies on Reaction Mechanism of CH3SO with NO

The potential energy surface （PES） of CH3SO radical with NO reaction has been studied at MP2/6-311G（2df, p） and QCISD/6-311G（2df, p） levels. Geometries of the reactants, transition states （TS） and products were optimized at B3LYP/6-311G （d,p） level. The geometries of the transition states were found for the first time. The calculated results show that the reaction can proceed via singlet-state or triplet-state PES. Because of the high energy barrier of triplet surface, the singlet surface reactions are dominant. The topological analysis of electron density shows that there are two kinds of structaral transition states （the bifurcation-type ring structure transition state and the T-shaped conflict structure transition state） in the titled reaction. The total electronic density of the reactants, TS and products and the spin electronic density on the triplet surface were also discussed in this paper.