High resolution infrared absorption spectra, crystal field, and relaxation processes in CsCdBr_3:Pr^3+

High resolution low-temperature absorption spectra of 0.2% Pr^3+ doped CsCdBr_3 were measured in the spectral region 2000--7000 cm-1. Positions and widths of the crystal field levels within the 3H5, 3H4, 3F2, and 3F3 multiplets of the Pr^3+ main center have been determined. Hyperfine structure of several spectral lines has been found. Crystal field calculations were carried out in the framework of the semiphenomenological exchange charge model (ECM). Parameters of the ECM were determined by fitting to the measured total splittings of the 3H4 and 3H6 multiplets and to the observed in this work hyperfine splittings of the crystal field levels. One- and two-phonon relaxation rates were calculated using the phonon Green's functions of the perfect (CsCdBr_3) and locally perturbed (impurity dimer centers in CsCdBr_3:Pr^3+) crystal lattice. Comparison with the measured linewidths confirmed an essential redistribution of the phonon density of states in CsCdBr_3 crystals doped with rare-earth ions.Comment: 16 pages, 5 tables, 3 figure

Optical spectra, crystal-field parameters, and magnetic susceptibility of the new multiferroic NdFe3(BO3)4

We report high-resolution optical absorption spectra for NdFe3(BO3)4 trigonal single crystal which is known to exhibit a giant magnetoelectric effect below the temperature of magnetic ordering TN = 33 K. The analysis of the temperature-dependent polarized spectra reveals the energies and, in some cases, symmetries and exchange splittings of Nd3+ 84 Kramers doublets. We perform crystal-field calculations starting from the exchange-charge model, obtain a set of six real crystal-field parameters, and calculate wave functions and magnetic g-factors. In particular, the values g(perpendicular) = 2.385, g(parallel) = 1.376 were found for the Nd3+ ground-state doublet. We obtain Bloc=7.88 T and |JFN|= 0.48 K for the values of the local effective magnetic field at liquid helium temperatures at the Nd3+ site and the Nd - Fe exchange integral, respectively, using the experimentally measured Nd3+ ground-state splitting of 8.8 cm-1. To check reliability of our set of crystal field parameters we model the magnetic susceptibility data from literature. A dimer containing two nearest-neighbor iron ions in the spiral chain is considered to partly account for quasi-one-dimensional properties of iron borates, and then the mean-field approximation is used. The results of calculations with the exchange parameters for Fe3+ ions Jnn = -6.25 K (intra-chain interactions) and Jnnn = -1.92 K (inter-chain interactions) obtained from fitting agree well with the experimental data.Comment: 13 pages, 8 figures, 2 table

Stark structure of the Yb3+ ion levels in (YbxY 1-x)2Ti2O7 and the crystal field in rare-earth titanates with a pyrochlore structure

The absorption spectra of Yb2Ti2O7 single crystals and the luminescence and luminescence excitation spectra of Y 2Ti2O7: Yb (1%) polycrystals were studied in the temperature range 4.2-300 K. The spectra were analyzed in terms of the crystal-field theory and the exchange-charge model. Based on the set of crystal-field parameters found for Yb2Ti2O7, analogous sets of parameters were determined for other rare-earth titanates and proved to be in reasonable agreement with all available experimental data. © 2005 Pleiades Publishing, Inc

Magnetization and specific heat of TbFe3(BO3)4: Experiment and crystal field calculations

We have studied the thermodynamic properties of single-crystalline TbFe3(BO3)4. Magnetization measurements have been carried out as a function of magnetic field (up to 50 T) and temperature up to 350K with the magnetic field both parallel and perpendicular to the trigonal c-axis of the crystal. The specific heat has been measured in the temperature range 2-300K with a magnetic field up to 9 T applied parallel to the c-axis. The data indicate a structural phase transition at 192 K and antiferromagnetic spin ordering at 40 K. A Schottky anomaly is present in the specific heat data around 20 K, arising due to two low-lying energy levels of the Tb3+ ions being split by f-d coupling. Below TN magnetic fields parallel to the c-axis drive a spin-flop phase transition, which is associated with a large magnetization jump. The highly anisotropic character of the magnetic susceptibility is ascribed mainly to the Ising-like behavior of the Tb3+ ions in the trigonal crystal field. We describe our results in the framework of an unified approach which is based on mean-field approximation and crystal-field calculations.Comment: 10 pages, 10 figures, 20 references, accepted by Phys. Rev.

Optical spectroscopy of Yb2Ti2O7 and Y2Ti2O7: Yb3+ and crystal-field parameters in rare-earth titanate pyrochlores

Optical absorption spectra of the Yb2Ti2O7 single crystals and luminescence spectra of the Y2Ti 2O7:Yb (1%) polycrystalline samples were registered at temperatures 4.2-300 K. These spectra and earlier published data on magnetic properties of Yb3+ ions and on the temperature dependence of the electric field gradient at Yb nuclei in Yb2Ti2O 7 were used to analyze the crystal-field parameters in rare-earth titanates with the pyrochlore structure. The self-consistent sets of crystal-field parameters for rare-earth ions in the 16d sites with the D 3d symmetry that describe satisfactory all known single-ion magnetic properties and low-energy excitations in R2Ti2O 7 crystals (R=Tb, Ho, Er, Tm, Yb) are presented

Lattice vibrations of alpha'-NaV_2O_5 in the low-temperature phase. Magnetic bound states?

We report high resolution polarized infrared studies of the quarter-filled spin ladder compound alpha'-NaV_2O_5 as a function of temperature (5K <= T <= 300K). Numerous new modes were detected below the temperature T_c=34K of the phase transition into a charge ordered nonmagnetic state accompanied by a lattice dimerization. We analyse the Brillouin zone (BZ) folding due to lattice dimerization at T_c and show that some peculiarities of the low-temperature vibrational spectrum come from quadruplets folded from the BZ point (1/2, 1/2, 1/4). We discuss an earlier interpretation of the 70, 107, and 133cm-1 modes as magnetic bound states and propose the alternative interpretation as folded phonon modes strongly interacting with charge and spin excitations.Comment: 15 pages, 13 Postscript figure

Stark structure of the Yb3+ ion levels in (YbxY 1-x)2Ti2O7 and the crystal field in rare-earth titanates with a pyrochlore structure

The absorption spectra of Yb2Ti2O7 single crystals and the luminescence and luminescence excitation spectra of Y 2Ti2O7: Yb (1%) polycrystals were studied in the temperature range 4.2-300 K. The spectra were analyzed in terms of the crystal-field theory and the exchange-charge model. Based on the set of crystal-field parameters found for Yb2Ti2O7, analogous sets of parameters were determined for other rare-earth titanates and proved to be in reasonable agreement with all available experimental data. © 2005 Pleiades Publishing, Inc

Stark structure of the Yb3+ ion levels in (YbxY 1-x)2Ti2O7 and the crystal field in rare-earth titanates with a pyrochlore structure

The absorption spectra of Yb2Ti2O7 single crystals and the luminescence and luminescence excitation spectra of Y 2Ti2O7: Yb (1%) polycrystals were studied in the temperature range 4.2-300 K. The spectra were analyzed in terms of the crystal-field theory and the exchange-charge model. Based on the set of crystal-field parameters found for Yb2Ti2O7, analogous sets of parameters were determined for other rare-earth titanates and proved to be in reasonable agreement with all available experimental data. © 2005 Pleiades Publishing, Inc

Optical spectroscopy of Yb2Ti2O7 and Y2Ti2O7: Yb3+ and crystal-field parameters in rare-earth titanate pyrochlores

Optical absorption spectra of the Yb2Ti2O7 single crystals and luminescence spectra of the Y2Ti 2O7:Yb (1%) polycrystalline samples were registered at temperatures 4.2-300 K. These spectra and earlier published data on magnetic properties of Yb3+ ions and on the temperature dependence of the electric field gradient at Yb nuclei in Yb2Ti2O 7 were used to analyze the crystal-field parameters in rare-earth titanates with the pyrochlore structure. The self-consistent sets of crystal-field parameters for rare-earth ions in the 16d sites with the D 3d symmetry that describe satisfactory all known single-ion magnetic properties and low-energy excitations in R2Ti2O 7 crystals (R=Tb, Ho, Er, Tm, Yb) are presented