The chromium spin density wave: magnetic X-ray scattering studies with polarisation analysis

We report on X-ray magnetic diffraction studies of the spin density wave antiferromagnetism formed in the conduction electron band of chromium. Non-resonant X-ray magnetic scattering was used to directly determine that chromium has zero orbital magnetisation. Furthermore, the azimuthal dependence of this scattering provides unique evidence that chromium forms a linearly polarised wave. In the vicinity of the K absorption edge, resonant X-ray magnetic scattering was observed. A consistent model of the magnetic scattering has been derived from the resonant and non-resonant magnetic amplitudes. The enhancement of the magnetic intensity arises primarily from dipole transitions from the core 1s level to 4p states. Quadrupole transitions to the magnetic 3d states are essentially non-existent due to their sensitivity to (and the absence of) orbital moment. This effect is predicted from atomic considerations of the 3d⁵ ( = 0) transition metal ions. Received 22 September 2000     

Femtosecond dynamics of the collinear-to-spiral antiferromagnetic phase transition in CuO

We report on the ultrafast dynamics of magnetic order in a single crystal of CuO at a temperature of 207 K in response to strong optical excitation using femtosecond resonant x-ray diffraction. In the experiment, a femtosecond laser pulse induces a sudden, nonequilibrium increase in magnetic disorder. After a short delay ranging from 400 fs to 2 ps, we observe changes in the relative intensity of the magnetic ordering diffraction peaks that indicate a shift from a collinear commensurate phase to a spiral incommensurate phase. These results indicate that the ultimate speed for this antiferromagnetic reorientation transition in CuO is limited by the long-wavelength magnetic excitation connecting the two phases.     

Soft X-ray resonant magnetic diffraction

We have conducted the first soft x-ray diffraction experiments from a bulk single crystal, studying the bilayer manganite La2-2xSr1+2xMn2O7 with x=0.475 in which we were able to access the (002) Bragg reflection using soft x rays. The Bragg reflection displays a strong resonant enhancement at the L(III) and L(II) manganese absorption edges. We demonstrate that the resonant enhancement of the magnetic diffraction of the (001) is extremely large, indeed so large that it exceeds that of the nonresonant Bragg diffraction. Resonant soft x-ray scattering of 3d transition metal oxides is the only technique for the atomic selective measurement of spin, charge, and orbital correlations in materials, such as high temperature superconductors, colossal magnetoresistance manganites, and charge stripe nickelates.     

Orbital ordering transition in Ca2RuO4 observed with resonant X-ray diffraction

Resonant x-ray diffraction performed at the L(II) and L(III) absorption edges of Ru has been used to investigate the magnetic and orbital ordering in Ca2RuO4 single crystals. A large resonant enhancement due to electric dipole 2p-->4d transitions is observed at the wave-vector characteristic of antiferromagnetic ordering. Besides the previously known antiferromagnetic phase transition at T(N)=110 K, an additional phase transition, between two paramagnetic phases, is observed around 260 K. Based on the polarization and azimuthal angle dependence of the diffraction signal, this transition can be attributed to orbital ordering of the Ru t(2g) electrons. The propagation vector of the orbital order is inconsistent with some theoretical predictions for the orbital state of Ca2RuO4.     

Orbital Ordering Effect on Magnetic Resonance Spectra in Charge-Ordered and Frustrated Manganites

Physics of the Solid State - A theoretical study of the interrelation of the crystal structure, charge, orbital, and magnetic subsystems in R1 – xAxMnO3 charge-ordered...     

Spin state transition in LaCoO3 studied using soft x-ray absorption spectroscopy and magnetic circular dichroism

Using soft x-ray absorption spectroscopy and magnetic circular dichroism at the Co-L(2,3) edge, we reveal that the spin state transition in LaCoO3 can be well described by a low-spin ground state and a triply degenerate high-spin first excited state. From the temperature dependence of the spectral line shapes, we find that LaCoO3 at finite temperatures is an inhomogeneous mixed-spin state system. It is crucial that the magnetic circular dichroism signal in the paramagnetic state carries a large orbital momentum. This directly shows that the currently accepted low- or intermediate-spin picture is at variance. Parameters derived from these spectroscopies fully explain existing magnetic susceptibility, electron spin resonance, and inelastic neutron data.     

Coupling between spin and orbital degrees of freedom in KCuF3

We present the results of resonant x-ray scattering experiments on KCuF3. Structurally forbidden reflections, corresponding to magnetic and 3d-orbital long-range order, have been observed. Integrated intensities have been measured as a function of incident energy, polarization, azimuthal angle, and temperature. The results give evidence for a strong coupling between orbital and spin degrees of freedom. The interplay between magnetic and orbital order parameters is revealed by the temperature dependence of the intensity of orbital Bragg peaks.     

Charge-Ordered Antiferromagnetic to Ferromagnetic Phase Transition in Cr-Doped Nd0.5Ca0.5Mn1−x Cr x O3: EMR and Magnetization Study

The Cr-doped rare-earth manganites Nd_0.5Ca_0.5Mn_1−x Cr _x O₃ (x = 0.03, 0.05, 0.10) are studied by electron magnetic resonance (EMR) and magnetization measurements in the paramagnetic as well as in the ferromagnetic phase. The magnetization measurements show that the charge-ordered antiferromagnetic phase decreases at the expense of ferromagnetic metallic phase and for Cr doping of x = 0.1, the charge-ordered phase melts completely. The EMR shows multiple signals for all three compositions in the ferromagnetic phase indicative of an anisotropic ferromagnetic phase. The difference between the shift of the high-field and low-field signals decreases with Cr doping, indicating that the magnetic anisotropy decreases with the Cr doping. In the paramagnetic phase the EMR line width follows Causa's model as observed in other colossal magnetoresistant manganites. Authors' address: Ajay Sharma, Department of Physics, Indian Institute of Science, Bangalore, India     

Effect of porosity on the permeability tensor of polycrystalline ferrites (independent grain approximation)

The effect of porosity on the form of the permeability tensor is calculated using the independent-grain approximation; this procedure is similar to the Schlömann method. The theoretical curve for the resonant-field distribution is approximated by the Lorentz curve using the method of least squares. It is shown that with this approximation, porosity increases the width of the ferromagnetic resonance line for a non-porous material by the width of the Lorentz distribution curve; thus the resonant field shifts toward lower values. Formulas are obtained for the resonant-field shift due to porosity and the broadening in the ferromagnetic resonance line; these formulas differ somewhat from the Schlömann formulas. In order to check the working formulas and the applicability of the independent-grain approximation, measurements were performed on the tensor for magnesium-chromium-copper ferrites with variable porosity and a magnetization on the order of 1200 gauss at a frequency of 4000 mHz. Specimens having the form of longitudinally magnetized circular cylinders were used so that there was no degeneration in uniform precession of magnetization with long spin waves. The observed effect of porosity on the width of the ferromagnetic resonance line (determined by measuring the tensor) was found to be in good quantitative agreement with calculation. The shift in the resonant field due to porosity was negligibly small, which also agreed with calculation. The experimental results show that when there is no degeneration in uniform precession with spin waves, the independent-grain approximation can be used in experiments even when the magnetization and resonant field are approximately equal.Here, we must allow for the static magnetic susceptibility in the formulas for the resonant-field shift and the broadening in the ferromagnetic resonance line.     

Determination of the mechanism for resonant scattering in LaMnO3

The resonant multiple Bragg x-ray diffraction is used to study the forbidden (104) reflection in LaMnO3. Using the interference between the three-beam scattering and resonant scattering we can determine the phase of the resonant scattering. This phase is shown to be consistent with a model in which the resonant scattering is caused by the influence of the Mn-O bond length distortion rather than directly by the orbital ordering on the Mn 4p band structure.     

Direct observation of antiferroquadrupolar ordering: resonant X-Ray scattering study of DyB2C2

Antiferroquadrupolar (AFQ) ordering has been conjectured in several rare-earth compounds to explain their anomalous magnetic properties. No direct evidence for AFQ ordering, however, has been reported. Using the resonant x-ray scattering technique near the Dy L(III) absorption edge, we have succeeded in observing the AFQ order parameter in DyB2C2 and analyzing the energy and polarization dependence. The much weaker coupling between the orbital degrees of freedom and the lattice in 4f electron systems than in 3d compounds makes them an ideal platform to study orbital interactions originating from electronic mechanisms.     

Magnetic order in the pseudogap phase of high-Tc superconductors

One of the leading issues in high-T(c) superconductors is the origin of the pseudogap phase in underdoped cuprates. Using polarized elastic neutron diffraction, we identify a novel magnetic order in the YB(2)Cu(3)O(6+) system. The observed magnetic order preserves translational symmetry of the lattice as proposed for orbital moments in the circulating current theory of the pseudogap state. To date, it is the first direct evidence of a hidden order parameter characterizing the pseudogap phase in high-T(c) cuprates.     

Jahn-teller dynamics in charge-ordered manganites from raman spectroscopy

The Raman spectra of the charge-ordered manganite Pr0.65Ca0.35MnO3 were studied as functions of temperature and excitation energy and compared to magnetic moment and electrical conductivity behaviors. Both the charge ordering ( T(co) approximately 225 K) and the antiferromagnetic transitions ( T(N) approximately 175 K) affect the spectral shape and intensity, indicating strong charge-lattice and spin-lattice couplings. Below T(co) a transition from dynamic Jahn-Teller distortions to a collective static distortion takes place. A change of the spectra is observed on increasing the excitation energy above 2.5 eV and it is attributed to a resonant polaron excitation.     

Oxygen stripes in La0.5Ca0.5MnO3 from ab initio calculations

We investigate the electronic, magnetic, and orbital properties of La0.5Ca0.5MnO3 perovskite by means of an ab initio electronic structure calculation within the Hartree-Fock approximation. Using the experimental crystal structure reported by Radaelli et al. [Phys. Rev. B 55, 3015 (1997)]], we find a charge-ordering stripelike ground state. The periodicity of the stripes, and the insulating magnetic structure, consisting of antiferromagnetically coupled zigzag chains, are in agreement with neutron x-ray and electron diffraction experiments. However, the detailed structure is more complex than that envisaged by simple models of charge and orbital order on Mn d levels alone, and is better described as a charge-density wave of oxygen holes, coupled to the Mn spin/orbital order.     

Two-spinon and orbital excitations of the spin-Peierls system TiOCl

We combine high-resolution resonant inelastic x-ray scattering with cluster calculations utilizing a recently derived effective magnetic scattering operator to analyze the polarization, excitation energy, and momentum-dependent excitation spectrum of the low-dimensional quantum magnet TiOCl in the range expected for orbital and magnetic excitations (0-2.5?eV). Ti 3d orbital excitations yield complete information on the temperature-dependent crystal-field splitting. In the spin-Peierls phase we observe a dispersive two-spinon excitation and estimate the inter- and intradimer magnetic exchange coupling from a comparison to cluster calculations.     

Spontaneous formation of vanadium "molecules" in a geometrically frustrated crystal: AlV2O4

We investigated the charge-ordered (CO) state in spinel AlV2O4 by electron diffraction, synchrotron x-ray diffraction, and magnetic measurements. It was found that the CO structure appearing below 700 K is characterized by the formation of V clusters (heptamers), each of which is consisting of 7 vanadium atoms and is in a spin-singlet state as a total. Theoretical consideration indicates that this unique molecularlike V heptamer is stabilized by a strong bonding of vanadium t(2g) orbitals.     

Photoinduced melting of antiferromagnetic order in La(0.5)Sr(1.5)MnO4 measured using ultrafast resonant soft x-ray diffraction

We used ultrafast resonant soft x-ray diffraction to probe the picosecond dynamics of spin and orbital order in La(0.5)Sr(1.5)MnO(4) after photoexcitation with a femtosecond pulse of 1.5 eV radiation. Complete melting of antiferromagnetic spin order is evidenced by the disappearance of a (1/4,1/4,1/2) diffraction peak. On the other hand, the (1/4,1/4,0) diffraction peak, reflecting orbital order, is only partially reduced. We interpret the results as evidence of destabilization in the short-range exchange pattern with no significant relaxation of the long-range Jahn-Teller distortions. Cluster calculations are used to analyze different possible magnetically ordered states in the long-lived metastable phase. Nonthermal coupling between light and magnetism emerges as a primary aspect of photoinduced phase transitions in manganites.     

6Li and 7li solid-state NMR spectroscopy of nitrogen ceramic phases

Two nitrogen ceramic phases, the oxynitride LiSiON and the nitride LiSi2N3, have been studied by 6Li and 7Li NMR. Magic angle spinning (MAS) NMR experiments have been carried out at two magnetic field strengths (7.05 and 14.1 T). The spectra give evidence of the relative effects of the quadrupolar and chemical shift interactions. The electric field gradient tensor of both phases has been determined accurately by iterative fitting of the 6Li and 7Li MAS NMR line shapes at the two magnetic field strengths. Due to the fact that for 7Li the quadrupolar interaction is much larger than the chemical shift interaction, it is shown that neither the small chemical shift anisotropy nor the relative orientation of the two interaction tensors can be determined accurately by 7Li MAS NMR. For 6Li, the two interactions are comparable and the value of these parameters obtained from the fits of the 6Li experimental MAS line shapes are therefore much more reliable.