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Inelastic neutron scattering studies of Crystal Field Levels in PrOs$_4$As$_{12}$

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 Added by Songxue Chi
 Publication date 2008
  fields Physics
and research's language is English




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We use neutron scattering to study the Pr$^{3+}$ crystalline electric field (CEF) excitations in the filled skutterudite PrOs$_4$As$_{12}$. By comparing the observed levels and their strengths under neutron excitation with the theoretical spectrum and neutron excitation intensities, we identify the Pr$^{3+}$ CEF levels, and show that the ground state is a magnetic $Gamma_4^{(2)}$ triplet, and the excited states $Gamma_1$, $Gamma_4^{(1)}$ and $Gamma_{23}$ are at 0.4, 13 and 23 meV, respectively. A comparison of the observed CEF levels in PrOs$_4$As$_{12}$ with the heavy fermion superconductor PrOs$_4$Sb$_{12}$ reveals the microscopic origin of the differences in the ground states of these two filled skutterudites.



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Comprehensive magnetic-field-orientation dependent studies of the susceptibility and de Haas-van Alphen effect have been carried out on single crystals of the filled skutterudites PrOs$_4$As$_{12}$ and LaOs$_4$As$_{12}$ using magnetic fields of up to 40~T. Several peaks are observed in the low-field susceptibility of PrOs$_4$As$_{12}$, corresponding to cascades of metamagnetic transitions separating the low-field antiferromagnetic and high-field paramagnetic metal (PMM) phases. The de Haas-van Alphen experiments show that the Fermi-surface topologies of PrOs$_4$As$_{12}$ in its PMM phase and LaOs$_4$As$_{12}$ are very similar. In addition, they are in reasonable agreement with the predictions of bandstructure calculations for LaOs$_4$As$_{12}$ on the PrOs$_4$As$_{12}$ lattice. Both observations suggest that the Pr 4$f$ electrons contribute little to the number of itinerant quasiparticles in the PMM phase. However, whilst the properties of LaOs$_4$As$_{12}$ suggest a conventional nonmagnetic Fermi liquid, the effects of direct exchange and electron correlations are detected in the PMM phase of PrOs$_4$As$_{12}$. For example, the quasiparticle effective masses in PrOs$_4$As$_{12}$ are found to decrease with increasing field, probably reflecting the gradual suppression of magnetic fluctuations associated with proximity to the low-temperature, low-field antiferromagnetic state.
Magnetization, specific heat, and electrical resistivity measurements were made on single crystals of the filled skutterudite compound PrOs$_{4}$As$_{12}$. Specific heat measurements indicate an electronic specific heat coefficient $gamma$ $sim 50-200$ mJ/mol K$^{2}$ at temperatures 10 K $leq T leq 18$ K, and $sim 1$ J/mol K$^{2}$ for $T leq 1.6$ K. Magnetization, specific heat, and electrical resistivity measurements reveal the presence of two, or possibly three, ordered phases at temperatures below $sim 2.3$ K and in fields below $sim 3$ T. The low temperature phase displays antiferromagnetic characteristics, while the nature of the ordering in the other phase(s) has yet to be determined.
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Emergence of an orbital-selective Mott phase (OSMP) found in multi-band correlated systems leads to a non-perturbative obliteration of the Landau Fermi liquid in favor of a novel metallic state exhibiting anomalous infra-red (branch-cut) continuum features in one- and two-particle responses. We use a combination of $(1)$ dynamical mean-field theory (DMFT) using the continuous-time-quantum Monte-Carlo (CTQMC) solver for a two-band Hubbard model and $(2)$ analytic arguments from an effective bosonized description to investigate strange metal features in inelastic neutron scattering studies for cuprates. Specifically, restricting our attention to symmetry-unbroken metallic phase, we study how emergence of an OSMP leads to qualitatively novel features in $(i)$ the dynamical spin and charge susceptibilities, and $(ii)$ phonon response in the strange metal, in detail. Extinction of the Landau quasiparticle pole in the one-electron propagator in the OSMP mirrors the emergence of critical liquid-like features in the dynamical spin response. This novel finding also underpins truly anomalous features in phonon dynamics, which we investigate by coupling half-breathing phonons in the specific context of cuprates to such a multi-electronic continuum. We find good understanding of various anomalies encountered in experimental inelastic neutron scattering studies in the near-optimally doped cuprates. We also extend these results in a phenomenological way to argue how modification of phonon spectra in underdoped cuprates can be reconciled with proposals for a nematic-plus-d-wave charge modulation order in the pseudogap state. We also study the issue of the dominant pair glue contributions to superconductivity, allowing us to interpret recent pump-probe results within a strange metal scenario.
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Inelastic neutron scattering experiments were performed to investigate the crystalline electric field (CEF) excitations of Nd3+ (J = 9/2) in the iron pnictide NdFeAsO. The crystal field level structures for both the high-temperature paramagnetic phase and the low-temperature antiferromagnetic phase of NdFeAsO are constructed. The variation of CEF excitations of Nd3+ reflects not only the change of local symmetry but also the change of magnetic ordered state of the Fe sublattice. By analyzing the crystal field interaction with a crystal field Hamiltonian, the crystal field parameters are obtained. It was found that the sign of the fourth and sixth-order crystal field parameters change upon the magnetic phase transition at 140 K, which may be due to the variation of exchange interactions between the 4f and conduction electrons.
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