Neptunium multipoles and resonant x-ray Bragg diffraction by neptunium dioxide (NpO2)

The low-temperature ordered state of neptunium dioxide (NpO(2)) remains enigmatic. After decades of experimental and theoretical efforts, long-range order of a time-odd (magnetic) high-order atomic multipole moment is now generally considered to be the fundamental order parameter, the most likely candidate being a magnetic triakontadipole (rank 5). To date, however, direct experimental observation of the primary order parameter remains outstanding. In the light of new experimental findings, we re-examine the effect of crystal symmetry on the atomic multipoles and the resulting x-ray resonant scattering signature. Our simulations use the crystallographic point group ?3m (D(3d)), because corresponding magnetic groups ?3m', ?3'm', and ?3'm are shown by us to be at odds with a wealth of experimental results. In addition to the previously observed (secondary) quadrupole order, we derive expressions for higher-order multipoles that might be observed in future experiments. In particular, magnetic octupole moments are predicted to contribute to Np M(2,3) and L(2,3) resonant scattering via E2–E2 events. The Lorentzian-squared lineshape observed at the M(4) resonance is shown to be the result of the anisotropy of the 3p(3/2) core levels. Quantitative comparison of our calculations to the measured data yields a core–hole width Γ = 2.60(7) eV and a core-state exchange energy [absolute value]ε(1/2)[absolute value] = 0.76(2) eV.     

酸根离子及其水溶液对镎酰离子结构性质的影响

利用B3LYP杂化密度泛函方法,在相对论有效芯势模型下,优化得到了NpO_2~(2+)离子及其配合物在气相和水溶液中的几何结构和电子结构,研究了NO-3、SO2-4和CO2-3离子及其水溶液对NpO_2~(2+)离子的结构和性质的影响.结果表明,NpO_2~(2+)离子结合各种酸根离子后其Np=O键的键长都有明显增长、Np和O原子的价电子轨道能均有升高,而考虑溶剂化效应后酸根离子的影响将减小.电荷分析发现,结合酸根离子后,NpO_2~(2+)中Np和O原子间形成的共价键的强度减弱、键长增长.对NpO_2~(2+)离子与三种酸根离子的理论结合能的比较显示,Np O2CO3分子最为稳定.     

酸根离子及其水溶液对镎酰离子结构性质的影响

利用B3LYP杂化密度泛函方法,在相对论有效芯势模型下,优化得到了NpO22+离子及其配合物在气相和水溶液中的几何结构和电子结构, 研究了NO3-、SO42-和CO32-离子及其水溶液对NpO22+离子的结构和性质的影响.结果表明,NpO22+离子结合各种酸根离子后其Np=O键的键长都有明显增长、Np和O原子的价电子轨道能均有升高,而考虑溶剂化效应后酸根离子的影响将减小.电荷分析发现,结合酸根离子后,NpO22+中Np和O原子间形成的共价键的强度减弱、键长增长.对NpO22+离子与三种酸根离子的理论结合能的比较显示,NpO2CO3分子最为稳定.     

Order parameter segregation in Ce0.7La0.3B6: 4f octopole and 5d dipole magnetic order

The intriguing thermophysical properties of CeB6 have been subject to investigation for more than 20 years. In particular, an exotic ground state, phase IV, emerges under doping with La. We report resonant x-ray scattering results on the order parameter symmetries in phase IV of Ce0.7La0.3B6, which condenses below T(IV)=1.5 K. The results reveal a degree of mesoscopic 5d dipole antiferromagnetic order, with propagation vector Q0=(1/2 1/2 1/2), both below and above T(IV). Below T(IV), this polarization coexists with long-range 4f antiferro-octupole (AFO) order also at Q0. The marked differences in temperature dependence and spatial correlation suggest a state of order parameter segregation at low temperature. A simple model of AFO order, consistent with the polarization dependent azimuth symmetries, the Bragg angle, and temperature dependence is given.     

镎氧化物分子结构和光谱的理论研究

运用密度泛函理论(DFT)的B3LYP方法,优化了NpO,NpO_2,NpO_3和Np_2O_3分子的几何构型,分析了电子从Np到O的转移情况。结果表明:NpO,NpO_2,NpO_3和Np_2O_3的自旋多重度分别为6,2,2和9,对称性分别为C_(∞v),D_(∞h),C_(2v)和D_(3h)时相应分子处于稳定结构;对所有分子而言,分子能级在-50 eV左右的态主要由Np-6s轨道形成,在-20 eV附近的态主要由Np-6p和O-2s轨道混合组成,而大于-11 eV的态主要由Np-5f和O-2p轨道混合组成。同时,根据相关计算给出了分子基态结构的振动频率和光谱数据,并对红外光谱最大峰值的振动模式进行了指认。     

Fragile magnetic ground state in half-doped LaSr2Mn2O7

We investigated the orbital and antiferromagnetic ordering behaviors of the half-doped bilayer manganite La(2-2x)Sr(1+2x)Mn2O7 (x ? 0.5) by using Mn L(2,3)-edge resonant soft x-ray scattering. Resonant soft x-ray scattering reveals the CE-type orbital order below T(oo) ? 220 K, which shows partial melting behavior below T(m) ? 165 K. We also found coexistence CE- and A-type antiferromagnetic orders. Both orders involve the CE-type orbital order with nearly the same orbital character and are coupled with each other. These results manifest that the ground state with the CE-type antiferromagnetic order is easily susceptible to destabilization into the A-type one even with a small fluctuation of the doping level, as suggested by the extremely narrow magnetic phase boundaries at x ? 0.5±0.005.     

Magnetic field enhancement of heat transport in the 2D Heisenberg antiferromagnet K2V3O8

The thermal conductivity and heat capacity of single crystals of the spin 1/2 quasi-2D Heisenberg antiferromagnet K(2)V(3)O(8) have been measured from 1.9 to 300 K in magnetic fields from 0 to 8 T. The zero field thermal conductivity data are consistent with resonant scattering of phonons by magnons near the zone boundary. Application of a magnetic field greater than 1 T, however, produces a new magnetic ground state with substantial heat transport by long wavelength magnons.     

NMR evidence for higher-order multipole order parameters in NpO2

We report a microscopic investigation of multipolar order parameters in the ordered state of NpO2 conducted via 17O NMR on a single crystal. From the angular dependence of hyperfine fields at 17O nuclei, we have obtained clear evidence for the appearance of field-induced antiferro-octupolar as well as field-induced antiferro-dipolar moments below T0 = 26 K. We have also observed oscillatory spin-echo decay, which is well understood in terms of small electric field gradients created by antiferro-quadrupolar ordering. This reveals that the quadrupolar order parameter is directly observable by means of NMR. The present NMR studies provide definitive support for a proposed longitudinal triple-q type octupolar-quadrupolar ordering model for NpO2.     

NMR evidence for triple-q multipole structure in NpO2

In order to elucidate the nature of the exotic ordered phase of NpO2 below T(0)=26 K, we have initiated the first 17O-NMR measurements on this system. From the 17O-NMR spectrum, the occurrence of two inequivalent oxygen sites has been confirmed below T0. It has also been shown that the characteristic features of the hyperfine interaction at the oxygen sites are well explained by invoking a hyperfine interaction with field-induced antiferromagnetic moments which appear as a result of the triple-q antiferroquadrupolar order. The NMR findings strongly support the occurrence of the longitudinal triple-q multipole structure in NpO2.     

Soft x-ray resonant diffraction study of magnetic and orbital correlations in a manganite near half doping

We have utilized resonant x-ray diffraction at the Mn L(II,III) edges in order to directly compare magnetic and orbital correlations in Pr0.6Ca0.4MnO3. Comparing the widths of the magnetic and orbital diffraction peaks, we find that the magnetic correlation length exceeds that of the orbital order by nearly a factor of 2. Furthermore, we observe a large (approximately 3 eV) spectral weight shift between the magnetic and orbital resonant line shapes, which cannot be explained within the classic Goodenough picture of a charge-ordered ground state. To explain the shift, we calculate the orbital and magnetic resonant diffraction line shapes based on a relaxed charge-ordered model.     

Resonant enhancement of inelastic light scattering in the fractional quantum Hall regime at ν=1/3

Strong resonant enhancements of inelastic light scattering from the long wavelength inter-Landau level magnetoplasmon and the intra-Landau level spin wave excitations are seen for the fractional quantum Hall state at ν=1/3. The energies of the sharp peaks (FWHM 0.2 meV) in the profiles of resonant enhancement of inelastic light scattering intensities coincide with the energies of photoluminescence bands assigned to negatively charged exciton recombination. To interpret the observed enhancement profiles, we propose three-step light scattering mechanisms in which the intermediate resonant transitions are to states with charged excitonic excitations.     

Direct determination of the magnetic ground state in the square lattice S = 1/2 antiferromagnet Li2VOSiO4

Powder neutron diffraction and resonant x-ray scattering measurements from a single crystal have been performed to study the low-temperature state of the 2D frustrated, quantum-Heisenberg system Li2VOSiO4. Both techniques indicate a collinear antiferromagnetic ground state, with propagation vector k=(1 / 2 1 / 2 0), and magnetic moments in the a-b plane. Contrary to previous reports, the ordered moment at 1.44 K, m=0.63(3)micro(B), is very close to the value expected for the square lattice Heisenberg model ( approximately 0.6micro(B)). The magnetic order is three dimensional, with antiferromagnetic a-b layers stacked ferromagnetically along the c axis. Neither x-ray nor neutron diffraction shows evidence for a structural distortion between 1.6 and 10 K.     

正常金属-铁磁绝缘层-dx2-y2+idxy混合波超导结中的磁散射对隧道谱的影响

在正常金属铁磁绝缘层dx2-y2 idxy混合波超导隧道结中,考虑到铁磁绝缘层的磁散射和界面的粗糙散射效应,运用BogoliubovdeGennes(BdG)方程和BlonderTinkhamKlapwijk(BTK)理论,计算了隧道结中的准粒子传输系数和微分电导.研究表明:(1)磁散射和界面粗糙散射均可以压低电导峰,其中磁散射能使电导峰滑移,而粗糙界面散射却能阻止这种滑移,且两散射的共同作用可抑制由混合波两序参数的幅值比不同所导致的电导峰滑移;(2)随铁磁层离超导表面距离的增加,隧道谱在零偏压处由凹陷变成了零偏压电导峰,继而又演化为凹陷中的中心峰;(3)当铁磁层离开超导表面有若干相干长度时,隧道谱中将呈现一些子能级谐振峰.     

Borromean three-body heteroatomic resonances

We present an approach to analyze recent experimental evidences of Efimov resonant states in mixtures of ultracold gases, by considering two-species three-body atomic systems bound in a Borromean configuration, where all the two-body interactions are unbound. For such Borromean three-body systems, it is shown that a continuum three-body s-wave resonance emerges from an Efimov state as a scattering length or a three-body scale is moved. The energy and width of the resonant state are determined from a scaling function with arguments given by dimension-less energy ratios relating the two-body virtual state subsystem energies with the shallowest three-body bound state. The peculiar behavior of such resonances is that their peaks are expected to move to lower values of the scattering length, with increasing width, as one raises the temperature. For Borromean systems, two resonant peaks are expected in ultralow-temperature regimes, which will disappear at higher energies. It is shown how a Borromean-Efimov excited bound state turns out to a resonant state by tuning the virtual two-body subsystem energies or scattering lengths, with all energies written in units of the next deeper shallowest Efimov state energy. The resonance position and width for the decay into the continuum are obtained as universal scaling functions (limit cycle) of the dimensionless ratios of the two and three-body scales, which are calculated numerically within a zero-range renormalized three-body model.     

Resonant enhancement of inelastic light scattering in strongly correlated materials

We use dynamical mean field theory to find an exact solution for inelastic light scattering in strongly correlated materials such as those near a quantum-critical metal-insulator transition. We evaluate the results for q=0 (Raman) scattering and find that resonant effects can be quite large, and yield a double resonance, a significant enhancement of nonresonant scattering peaks, a joint resonance of both peaks when the incident photon frequency is on the order of U, and the appearance of an isosbestic point in all symmetry channels for an intermediate range of incident photon frequencies.     

Role of final states in photoemission from Al(1 1 1)

Enhancement of surface state peaks in angle resolved ultraviolet photoelectron spectra (ARUPS) from the Al(1 1 1) surface is studied experimentally and theoretically within the one-step model of photoemission. The resonant enhancement of the surface state emission is explained by the crucial role of elastic scattering of the outgoing electron. Dipole transitions to evanescent states in the final bands of the crystal are shown to determine photoemission at the resonant photon energy. The band structure based explanation is confirmed by the measurements of electron reflectivity and of the fine structure of valence band spectra. The surface sensitivity of ARUPS is shown to depend strongly on the complex band structure of the crystal and to be finely tunable by the choice of photoemitted electron energy.     

Spin waves and quantum criticality in the frustrated XY pyrochlore antiferromagnet Er2Ti2O7

We report detailed measurements of the low temperature magnetic phase diagram of Er2Ti2O7. Heat capacity and time-of-flight neutron scattering studies of single crystals reveal unconventional low-energy states. Er3+ magnetic ions reside on a pyrochlore lattice in Er2Ti2O7, where local XY anisotropy and antiferromagnetic interactions give rise to a unique frustrated system. In zero field, the ground state exhibits coexisting short and long-range order, accompanied by soft collective spin excitations previously believed to be absent. The application of finite magnetic fields tunes the ground state continuously through a landscape of noncollinear phases, divided by a zero temperature phase transition at micro{0}H{c} approximately 1.5 T. The characteristic energy scale for spin fluctuations is seen to vanish at the critical point, as expected for a second order quantum phase transition driven by quantum fluctuations.     

Quantum spin fluctuations in the spin-liquid state of Tb?Ti?O?

Neutron scattering experiments on a polycrystalline sample of the frustrated pyrochlore magnet Tb(2)Ti(2)O(7), which does not show any magnetic order down to 50 mK, have revealed that it shows condensation behavior below 0.4 K from a thermally fluctuating paramagnetic state to a spin-liquid ground state with quantum spin fluctuations. Energy spectra change from quasielastic scattering to a continuum with a double-peak structure at energies of 0 and 0.8 K in the spin-liquid state. Specific heat shows an anomaly at the crossover temperature.     

Photoassociative spectroscopy as a self-sufficient tool for the determination of the Cs triplet scattering length

In photoassociation spectroscopy, the line intensities of a given vibrational progression exhibit zero-signal modulation reflecting the node structure of the s-wave ground state wave function of two free colliding atoms. This leads to the determination of the scattering length. We performed photoassociation of cold Cs atoms polarized in the Zeeman sublevel f = 4, m(f) = 4. We analyzed the intensities of the lines associated with the Cs2 0(-)(g) state dissociating to the 6s(1/2)+6p(3/2) asymptote. This yields a value of the Cs triplet state scattering length, a(T) = -530a(0), while consistency requirements impose a value of the multipole ground state molecular coefficient, C6 = 6510 a.u.     

Magnetic resonant mode in the low-energy spin-excitation spectrum of superconducting Rb2Fe4Se5 single crystals

We have studied the low-energy spin-excitation spectrum of the single-crystalline Rb(2)Fe(4)Se(5) superconductor (T(c)=32 K) by means of inelastic neutron scattering. In the superconducting state, we observe a magnetic resonant mode centered at an energy of ?ω(res)=14 meV and at the (0.5 0.25 0.5) wave vector (unfolded Fe-sublattice notation), which differs from the ones characterizing magnetic resonant modes in other iron-based superconductors. Our finding suggests that the 245-iron selenides are unconventional superconductors with a sign-changing order parameter, in which bulk superconductivity coexists with the √5×√5 magnetic superstructure. The estimated ratios of ?ω(res)/k(B)T(c)≈5.1±0.4 and ?ω(res)/2Δ≈0.7±0.1, where Δ is the superconducting gap, indicate moderate pairing strength in this compound, similar to that in optimally doped 1111 and 122 pnictides.