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Register a new userAtomic multiplet calculation of 3d_{5/2} -> 4f resonant x-ray diffraction from Ho metal
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We compare for Ho metal the x-ray absorption spectrum and the resonant soft x-ray diffraction spectra obtained at the $3d_{5/2} to 4f$ ($M_5$) resonance for the magnetic 1st and 2nd order diffraction peaks $(0,0,tau)$ and $(0,0,2tau)$ with the result of an atomic multiplet calculation. We find a good agreement between experiment and simulation giving evidence that this kind of simulation is well suited to quantitatively analyze resonant soft x-ray diffraction data from correlated electron systems.
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CeB6, a typical Gamma_8-quartet system, exhibits a mysterious antiferroquadrupolar ordered phase in magnetic fields, which is considered as originating from the T_{xyz}-type magnetic octupole moment induced by the field. By resonant x-ray diffraction in magnetic fields, we have verified that the T_{xyz}-type octupole is indeed induced in the 4f-orbital of Ce with a propagation vector (1/2, 1/2, 1/2), thereby supporting the theory. We observed an asymmetric field dependence of the intensity for an electric quadrupole (E2) resonance when the field was reversed, and extracted a field dependence of the octupole by utilizing the interference with an electric dipole (E1) resonance. The result is in good agreement with that of the NMR-line splitting, which reflects the transferred hyperfine field at the Boron nucleus from the anisotropic spin distribution of Ce with an O_{xy}-type quadrupole. The field-reversal method used in the present study opens up the possibility of being widely applied to other multipole ordering systems such as NpO2, Ce_{x}La_{1-x}B_{6}, SmRu_{4}P_{12}, and so on.
Soft resonant x-ray Bragg diffraction (SRXD) at the Ho M$_{4,5}$ edges has been used to study Ho $4f$ multipoles in the combined magnetic and orbitally ordered phase of HoB$_2$C$_2$. A full description of the energy dependence for both $sigma$ and $pi$ incident x-rays at two different azimuthal angles, as well as the ratio $I_sigma/I_pi$ as a function of azimuthal angle for a selection of energies, allows a determination of the higher order multipole moments of rank 1 (dipole) to 6 (hexacontatetrapole). The Ho 4f multipole moments have been estimated, indicating a dominant hexadecapole (rank 4) order with an almost negligible influence from either the dipole or the octupole magnetic terms. The analysis incorporates both the intra-atomic magnetic and quadrupolar interactions between the 3d core and 4f valence shells as well as the interference of contributions to the scattering that behave differently under time reversal. Comparison of SRXD, neutron diffraction and non resonant x-ray diffraction shows that the magnetic and quadrupolar order parameter are distinct. The $(0 0 1/2)$ component of the magnetic order exhibits a Brillouin type increase below the orbital ordering temperature T$_Q$, while the quadrupolar order increases more sharply. We conclude the quadrupolar interaction is strong, but quadrupolar order only occurs when the magnetic order gives rise to a quasi doublet ground state, which results in a lock-in of the orbitals at T$_Q$.
The magnetic structure and fluctuations of tetragonal GdRhIn5 were studied by resonant x-ray diffraction at the Gd LII and LIII edges, followed by a renormalization group analysis for this and other related Gd-based compounds, namely Gd2IrIn8 and GdIn3. These compounds are spin-only analogs of the isostructural Ce-based heavy-fermion superconductors. The ground state of GdRhIn5 shows a commensurate antiferromagnetic spin structure with propagation vector tau = (0,1/2, 1/2), corresponding to a parallel spin alignment along the a-direction and antiparallel alignment along b and c. A comparison between this magnetic structure and those of other members of the Rm(Co,Rh,Ir)n In3m+2n family (R =rare earth, n = 0, 1; m = 1, 2) indicates that, in general, tau is determined by a competition between first-(J1) and second-neighbor(J2) antiferromagnetic (AFM) interactions. While a large J1 /J2 ratio favors an antiparallel alignment along the three directions (the so-called G-AFM structure), a smaller ratio favors the magnetic structure of GdRhIn5 (C-AFM). In particular, it is inferred that the heavy-fermion superconductor CeRhIn5 is in a frontier between these two ground states, which may explain its non-collinear spiral magnetic structure. The critical behavior of GdRhIn5 close to the paramagnetic transition at TN = 39 K was also studied in detail. A typical second-order transition with the ordered magnetization critical parameter beta = 0.35 was experimentally found, and theoretically investigated by means of a renormalization group analysis.
X-ray resonant scattering has been used to measure the magnetic order of the Dy ions below 40K in multiferroic DyMn$_{2}$O$_{5}$. The magnetic order has a complex behaviour. There are several different ordering wavevectors, both incommensurate and commensurate, as the temperature is varied. In addition a non-magnetic signal at twice the wavevector of one of the commensurate signals is observed, the maximum intensity of which occurs at the same temperature as a local maximum in the ferroelectric polarisation. Some of the results, which bear resemblence to the behaviour of other members of the RMn$_{2}$O$_{5}$ family of multiferroic materials, may be explained by a theory based on so-called acentric spin-density waves.
The distribution of chemically similar transition-metal ions is a fundamental issue in the study of herbertsmithite-type kagome antiferromagnets. Using synchrotron radiation, we have performed resonant powder x-ray diffractions on newly synthesized CoCu3(OH)6Cl2, which provide an exact distribution of transition-metal ions in the frustrated antiferromagnet. Both magnetic susceptibility and specific heat measurements are quantitatively consistent with the occupation fractions determined by resonant x-ray diffraction. The distribution of transition-metal ions and residual magnetic entropy suggest a novel low temperature (T < 4 K) magnetism, where the interlayer triangular spins undergo a spin-glass freezing while the kagome spins still keep highly frustrated.
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