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Register a new userPrecise determination of low energy electronuclear Hamiltonian for LiY$_{1-x}$Ho$_{x}$F$_{4}$
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We use complementary optical spectroscopy methods to directly measure the lowest crystal-field energies of the rare-earth quantum magnet LiY$_{1-x}$Ho$_{x}$F$_{4}$, including their hyperfine splittings, with more than 10 times higher resolution than previous work. We are able to observe energy level splittings due to the $^6mathrm{Li}$ and $^7mathrm{Li}$ isotopes, as well as non-equidistantly spaced hyperfine transitions originating from dipolar and quadrupolar hyperfine interactions. We provide refined crystal field parameters and extract the dipolar and quadrupolar hyperfine constants ${A_J=0.02703pm0.00003}$ $textrm{cm}^{-1}$ and ${B= 0.04 pm0.01}$ $textrm{cm}^{-1}$, respectively. Thereupon we determine all crystal-field energy levels and magnetic moments of the $^5I_8$ ground state manifold, including the (non-linear) hyperfine corrections. The latter match the measurement-based estimates. The scale of the non-linear hyperfine corrections sets an upper bound for the inhomogeneous line widths that would still allow for unique addressing of a selected hyperfine transition. e.g. for quantum information applications. Additionally, we establish the far-infrared, low-temperature refractive index of LiY$_{1-x}$Ho$_{x}$F$_{4}$.
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We present zero-field {mu}SR measurements for LiY$_{1-x}$Ho$_{x}$F$_{4}$ samples with x = 0.0017, 0.0085, 0.0406, and 0.0855. We characterize the dynamics associated with the formation of the (F-{mu}-F)$^{-1}$ complex by comparing our data to Monte Carlo simulations to determine the concentration range over which the spin dynamics are determined primarily by the Ho$^{3+}$-{mu} interaction rather than the F-{mu} interaction. Simulations show that F-{mu}-F oscillations should evolve into a Lorentzian Kubo-Toyabe decay for an increasing static magnetic field distribution {Gamma} (i.e., increasing x), but the data do not show this behavior, consistent with the recently reported existence of strong magnetic fluctuations in this system at low temperatures. Anisotropy in the field distribution is shown to cause small errors of order 10% from behavior predicted for an isotropic distribution. Finally, numerical calculations show that values of {Gamma} calculated in the single ion limit greatly exceed the values extracted from curve fits, suggesting that strong correlations play an important role in this system.
We present measurements of magnetic field and frequency dependences of the low temperature (T = 1.8 K) AC-susceptibility, and temperature and field dependences of the longitudinal field positive muon spin relaxation ({mu}SR) for LiY$_{1-x}$Ho$_x$F$_4$ with x = 0.0017, 0.0085, 0.0408, and 0.0855. The fits of numerical simulations to the susceptibility data for the x = 0.0017, 0.0085 and 0.0408 show that Ho-Ho cross-relaxation processes become more important at higher concentrations, signaling the crossover from single-ion to correlated behavior. We simulate the muon spin depolarization using the parameters extracted from the susceptibility, and the simulations agree well with our data for samples with x = 0.0017 and 0.0085. The {mu}SR data for samples with x = 0.0408 and 0.0855 at low temperatures (T < 10 K) cannot be described within a single-ion picture of magnetic field fluctuations and give evidence for additional mechanisms of depolarization due to Ho$^{3+}$ correlations. We also observe an unusual peak in the magnetic field dependence of the muon relaxation rate in the temperature interval 10 - 20 K that we ascribe to a modification of the Ho$^{3+}$ fluctuation rate due to a field induced shift of the energy gap between the ground and the first excited doublet crystal field states relative to a peak in the phonon density of states centered near 63 cm$^{-1}$.
Raman spectra have been measured on iron-based quaternary CeO$_{1-x}$F$_x$FeAs and LaO$_{1-x}$F$_x$FeAs with varying fluorine doping at room temperatures. A group analysis has been made to clarify the optical modes. Based on the first principle calculations, the observed phonon modes can be assigned accordingly. In LaO$_{1-x}$F$_x$FeAs, the E$_g$ and A$_{1g}$ modes related to the vibrations of La, are suppressed with increasing F doping. However F doping only has a small effect on the E$_g$ and A$_{1g}$ modes of Fe and As. The Raman modes of La and As are absent in rare-earth substituted CeO$_{1-x}$F$_x$FeAs, and the E$_g$ mode of oxygen, corresponding to the in-plane vibration of oxygen, moves to around 450 cm$^{-1}$ and shows a very sharp peak. Electronic scattering background is low and electron-phonon coupling is not evident for the observed phonon modes. Three features are found above 500 cm$^{-1}$, which may be associated with multi-phonon process. Nevertheless it is also possible that they are related to magnetic fluctuations or interband transitions of d orbitals considering their energies.
Hall effect and magnetoresistance have been measured on single crystals of $NdFeAsO_{1-x}F_{x}$ with x = 0 ($T_c$ = 0 $ $K) and x = 0.18 ($T_c$ = 50 $ $K). For the undoped samples, strong Hall effect and magnetoresistance with strong temperature dependence were found below about 150 K. The magnetoresistance was found to be as large as 30% at 15 K at a magnetic field of 9 T. From the transport data we found that the transition near 155 K was accomplished in two steps: first one occurs at 155 K which may be associated with the structural transition, the second one takes place at about 140 K which may correspond to the spin-density wave like transition. In the superconducting sample with $T_c$ = 50 $ $K, it is found that the Hall coefficient also reveals a strong temperature dependence with a negative sign. But the magnetoresistance becomes very weak and does not satisfy the Kohlers scaling law. These dilemmatic results (strong Hall effect and very weak magnetoresistance) prevent to understand the normal state electric conduction by a simple multi-band model by taking account the electron and hole pockets. Detailed analysis further indicates that the strong temperature dependence of $R_H$ cannot be easily understood with the simple multi-band model either. A picture concerning a suppression to the density of states at the Fermi energy in lowering temperature is more reasonable. A comparison between the Hall coefficient of the undoped sample and the superconducting sample suggests that the doping may remove the nesting condition for the formation of the SDW order, since both samples have very similar temperature dependence above 175 K.
We report density functional theory calculations for the parent compound LaOFeAs of the newly discovered 26K Fe-based superconductor LaO$_{1-x}$F$_x$FeAs. We find that the ground state is an ordered antiferromagnet, with staggered moment about 2.3$mu_B$, on the border with the Mott insulating state. We fit the bands crossing the Fermi surface, derived from Fe and As, to a tight-binding Hamiltonian using maximally localized Wannier functions on Fe 3d and As 4p orbitals. The model Hamiltonian accurately describes the Fermi surface obtained via first-principles calculations. Due to the evident proximity of superconductivity to antiferromagnetism and the Mott transition, we suggest that the system may be an analog of the electron doped cuprates, where antiferromagnetism and superconductivity coexist.
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