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Register a new userf-Electron-Nuclear Hyperfine-Coupled Multiplets in the Unconventional Charge Order Phase of Filled Skutterudite PrRu4P12
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In the unconventional f-electron-associated charge order phase of filled skutterudite PrRu4P12, the low-temperature behaviors of the triplet crystalline-electric-field ground state of Pr ions have been studied by specific heat and magnetization measurements using high quality single crystals. Specific heat shows an anomalous Schottky-type peak structure at 0.30 K in zero field in spite of the absence of any symmetry breaking. Magnetization curve at 0.06 K shows a remarkable rounding below 1 T. It has been revealed that these anomalies provide compelling evidence for the formation of a lattice of Pr 4f-electron-nuclear hyperfine-coupled multiplets, the first known thermodynamical observation of its kind.
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We report the de Haas-van Alphen (dHvA) effect and magnetoresistance in the filled-skutterudite superconductor LaRu4P12, which is a reference material of PrRu4P12 that exhibits a metal-insulator (M-I) transition at T_MI~60 K. The observed dHvA branches for the main Fermi surface (FS) are well explained by the band-structure calculation, using the full potential linearized augmented-plane-wave method with the local-density approximation, suggesting a nesting instability with q =(1,0,0) in the main multiply connected FS as expected also in PrRu4P12. Observed cyclotron effective masses of (2.6-11.8)m_0, which are roughly twice the calculated masses, indicate the large mass enhancement even in the La-skutterudites. Comparing the FS between LaRu4P12 and PrRu4P12, an essential role of c-f hybridization cooperating with the FS nesting in driving the the M-I transition in PrRu4P12 has been clarified.
We report a novel insulator-insulator transition arising from the internal charge degrees of freedom in the two-dimensional quarter-filled organic salt beta-(meso-DMBEDT-TTF)2PF6. The optical conductivity spectra above Tc = 70 K display a prominent feature of the dimer-Mott insulator, characterized by a substantial growth of a dimer peak near 0.6 eV with decreasing temperature. The dimer-peak growth is rapidly quenched as soon as a peak of the charge order shows up below Tc, indicating a competition between the two insulating phases. Our infrared imaging spectroscopy has further revealed a spatially competitive electronic phases far below Tc, suggesting a nature of quantum phase transition driven by material-parameter variations.
We present a comprehensive study of the effect of hydrostatic pressure on the magnetic structure and spin dynamics in the spin-1/2 coupled ladder compound C$_9$H$_{18}$N$_2$CuBr$_4$. The applied pressure is demonstrated as a parameter to effectively tune the exchange interactions in the spin Hamiltonian without inducing a structural transition. The single-crystal heat capacity and neutron diffraction measurements reveal that the N$rm acute{e}$el ordered state breaks down at and above a critical pressure $P_{rm c}$$sim$1.0 GPa through a continuous quantum phase transition. The thorough analysis of the critical exponents indicates that such transition with a large anomalous exponent $eta$ into a quantum-disordered state cannot be described by the classic Landaus paradigm. Using inelastic neutron scattering and quantum Monte Carlo methods, the high-pressure regime is proposed as a $Z_2$ quantum spin liquid phase in terms of characteristic fully gapped vison-like and fractionalized excitations in distinct scattering channels.
The nature of order in low-temperature phases of some materials is not directly seen by experiment. Such hidden orders (HO) may inspire decades of research to identify the mechanism underlying those exotic states of matter. In insulators, HO phases originate in degenerate many-electron states on localized f or d shells that may harbor high-rank multipole moments. Coupled by inter-site exchange, those moments form a vast space of competing order parameters. Here, we show how the ground state order and magnetic excitations of a prototypical HO system, neptunium dioxide NpO$_2$, can be fully described by a low-energy Hamiltonian derived by a many-body ab initio force-theorem method. Superexchange interactions between the lowest crystal-field quadruplet of Np$^{4+}$ ions induce a primary non-collinear order of time-odd rank-5 (triakontadipolar) moments with a secondary quadrupole order preserving the cubic symmetry of NpO$_2$. Our study also reveals an unconventional multipolar exchange-striction mechanism behind the anomalous volume contraction of the NpO$_2$ HO phase.
A typical f-electron Kondo lattice system Ce exhibits the well-known isostructural transition, the so-called gamma-alpha transition, accompanied by an enormous volume collapse. Most interestingly, we have discovered that a topological-phase transition also takes place in elemental Ce, concurrently with the gamma-alpha transition. Based on the dynamical mean-field theory approach combined with density functional theory, we have unravelled that the non-trivial topology in alpha-Ce is driven by the f-d band inversion, which arises from the formation of coherent 4f band around the Fermi level. We captured the formation of the 4f quasi-particle band that is responsible for the Lifshitz transition and the non-trivial Z2 topology establishment across the phase boundary. This discovery provides a concept of topology switch for topological Kondo systems. The on and off switching knob in Ce is versatile in a sense that it is controlled by available pressure (around 1 GPa) at room temperature.
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