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Neutron spectroscopic study of crystal-field excitations and the effect of the crystal field on dipolar magnetism in Li$R$F$_4$ ($R$ = Gd, Ho, Er, Tm, and Yb)

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 Added by Peter Babkevich
 Publication date 2015
  fields Physics
and research's language is English




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We present a systematic study of the crystal field interactions in the Li$R$F$_4$, $R$ = Gd, Ho, Er, Tm and Yb, family of rare-earth magnets. Using detailed inelastic neutron scattering measurements we have been able to quantify the transition energies and wavefunctions for each system. This allows us to quantitatively describe the high-temperature susceptibility measurements for the series of materials and make predictions based on a mean-field approach for the low-temperature thermal and quantum phase transitions. We show that coupling between crystal field and phonon states leads to lineshape broadening in LiTmF$_4$ and level splitting in LiYbF$_4$. Furthermore, using high resolution neutron scattering from LiHoF$_4$, we find anomalous broadening of crystal-field excitations which we attribute to magnetoelastic coupling.



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The magnetic phase diagrams of RMnO3 (R = Er, Yb, Tm, Ho) are investigated up to 14 Tesla via magnetic and dielectric measurements. The stability range of the AFM order below the Neel temperature of the studied RMnO3 extends to far higher magnetic fields than previously assumed. Magnetic irreversibility indicating the presence of a spontaneous magnetic moment is found near 50 K for R=Er, Yb, and Tm. At very low temperatures and low magnetic fields the phase boundary defined by the ordering of the rare earth moments is resolved. The sizable dielectric anomalies observed along all phase boundaries are evidence for strong spin-lattice coupling in the hexagonal RMnO3. In HoMnO3 the strong magnetoelastic distortions are investigated in more detail via magnetostriction experiments up to 14 Tesla. The results are discussed based on existing data on magnetic symmetries and the interactions between the Mn-spins, the rare earth moments, and the lattice.
The magnetoelectric effect in the system $RAl_3(BO_3)_4$ ($R$ = Tb, Ho, Er, Tm) is investigated between 3 K and room temperature and at magnetic fields up to 70 kOe. We show a systematic increase of the magnetoelectric effect with decreasing magnetic anisotropy of the rare earth moment. A giant magnetoelectric polarization is found in the magnetically (nearly) isotropic $HoAl_3(BO_3)_4$. The polarization value in transverse field geometry at 70 kOe reaches 3600 $mu C/m^2$ which is significantly higher than reported values for the field-induced polarization of linear magnetoelectric or even multiferroic compounds. The results indicate a very strong coupling of the f-moments to the lattice. They further indicate the importance of the field-induced ionic displacements in the unit cell resulting in a polar distortion and a change in symmetry on a microscopic scale. The system $RAl_3(BO_3)_4$ could be interesting for the technological utilization of the high-field magnetoelectric effect.
The borocarbides RNi2B2C (R=Gd, Ho, Er) exhibit a large variety of magnetic states and as a consequence rich phase diagrams. We have analyzed the nature of these states by specific heat investigations. The data were measured down to 0.5 K and up to 80 kOe. The overall evolution of each Cm(T,H) curve is observed to reflect faithfully the features of the corresponding H-T phase diagram. Within the lower ranges of temperature and fields, the calculations based on linearized field-dependent spin-wave theory are found to reproduce satisfactorily the measured Cm(T,H) curves: accordingly, within these ranges, the thermodynamical properties of these compounds can be rationalized in terms of only two parameters: the spin-wave energy gap and the stiffness coefficient. For the intermediate fields ranges (H1<H<Hsat) wherein successive field-induced metamagnetic modes are stabilized, the evolution of Cm(T,H) is discussed in terms of the Maxwell relation (dCm/dH)T=T(d^2M/dT^2)H. For the particular case of GdNi2B2C wherein the anisotropy is dictated by the classical dipole interaction, Cm(T,H) across the whole ordered state is numerically evaluated within the model of Jensen and Rotter [PRB 77 (2008) 134408].
The antiferromagnetic transition is investigated in the rare-earth (R) tritelluride RTe3 family of charge density wave (CDW) compounds via specific heat, magnetization and resistivity measurements. Observation of the opening of a superzone gap in the resistivity of DyTe3 indicates that additional nesting of the reconstructed Fermi surface in the CDW state plays an important role in determining the magnetic structure.
We report the results of our investigation of the physical properties of mixed metal oxides RFe0.5Cr0.5O3 (R = Er and Yb). ErFe0.5Cr0.5O3 undergoes an antiferromagnetic ordering around 270 K followed by spin reorientation (SR) transitions around 150 and 8 K respectively. In contrast, in YbFe0.5Cr0.5O3 a single SR transition is noted at 36 K, below the AFM ordering temperature of 280 K. In ErFe0.5Cr0.5O3, a significant value of magnetic entropy change ({Delta}SM) ~ -12.4 J/kg-K is noted near the 2nd SR transition, however, this value is suppressed in YbFe0.5Cr0.5O3. Temperature dependent dielectric permittivity of ErFe0.5Cr0.5O3 and YbFe0.5Cr0.5O3 at different frequencies, reveal the presence of Debye-like relaxation behaviour in both compounds, which can be due to the effect of charge carrier hopping between localized states of Fe and Cr ions. Temperature dependent Raman scattering studies divulge that spin-phonon coupling plays a crucial role in defining the physical properties of these compounds.
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