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Register a new userMetal-to-metal transition and heavy-electron state in Nd$_4$Ni$_3$O$_{10-delta}$
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The trilayer nickelate Nd$_4$Ni$_3$O$_{10-delta}$ ($delta approx$ 0.15) was investigated by the measurements of x-ray diffraction, electrical resistivity, magnetic susceptibility, and heat capacity. The crystal structure data suggest a higher Ni valence in the inner perovskite-like layer. At ambient pressure the resistivity shows a jump at 162 K, indicating a metal-to-metal transition (MMT). The MMT is also characterized by a magnetic susceptibility drop, a sharp specific-heat peak, and an isotropic lattice contraction. Below $sim$ 50 K, a resistivity upturn with a log$T$ dependence shows up, accompanying with a negative thermal expansion. External hydrostatic pressure suppresses the resistivity jump progressively, coincident with the diminution of the log$T$ behavior. The low-temperature electronic specific-heat coefficient is extracted to be $sim$ 150 mJ K$^{-2}$ mol-fu$^{-1}$, equivalent to $sim$ 50 mJ K$^{-2}$ mol-Ni$^{-1}$, indicating an unusual heavy-electron correlated state. The novel heavy-electron state as well as the logarithmic temperature dependence of resistivity is explained in terms of the Ni$^{3+}$ centered Kondo effect in the inner layer of the (NdNiO$_3$)$_3$ trilayers.
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As a member of the Ruddlesden-Popper Ln$_{n+1}$Ni$_n$O$_{3n+1}$ series rare-earth-nickelates, the Pr4Ni$_3$O$_{10}$ consists of infinite quasi-two-dimensional perovskite-like Ni-O based layers. Although a metal-to-metal phase transition at Tpt = 157 K has been revealed by previous studies, a comprehensive study of physical properties associated with this transition has not yet been performed. We have grown single crystals of Pr4Ni3O10 at high oxygen pressure, and report on the physical properties around that phase transition, such as heat-capacity, electric-transport and magnetization. We observe a distinctly anisotropic behavior between in-plane and out-of-plane properties: a metal-to-metal transition at Tpt within the a-b plane, and a metal-to-insulator-like transition along the c-axis with decreasing temperature. Moreover, an anisotropic and anomalous negative magneto-resistance is observed at Tpt that we attribute to a slight suppression of the first-order transition with magnetic field. The magnetic-susceptibility can be well described by a Curie-Weiss law, with different Curie-constants and Pauli-spin susceptibilities between the high-temperature and the low-temperature phases. The single crystal X-ray diffraction measurements show a shape variation of the different NiO6 octahedra from the high-temperature phase to the low-temperature phase. This subtle change of the environment of the Ni sites is likely responsible for the different physical properties at high and low temperatures.
We study the many-body electronic structure of the stoichiometric and electron-doped trilayer nickelate Pr$_4$Ni$_3$O$_8$ in comparison to that of the stoichiometric and hole-doped infinite layer nickelate NdNiO$_2$ within the framework of density functional plus dynamical mean field theory, noting that Pr$_4$Ni$_3$O$_8$ has the same nominal carrier concentration as NdNiO$_2$ doped to a level of 1/3 holes/Ni. We find that the correlated Ni-$3d$ shells of both of these low valence nickelates have similar many-body configurations with correlations dominated by the $d_{x^2-y^2}$ orbital. Additionally, when compared at the same nominal carrier concentration, the materials exhibit similar many-body electronic structures, self energies, and correlation strengths. Compared to cuprates, these materials are closer to the Mott-Hubbard regime due to their larger charge transfer energies. Moreover, doping involves the charge reservoir provided by the rare earth $5d$ electrons, as opposed to cuprates where it is realized via the oxygen $2p$ electrons.
Ab initio calculations have been performed to unravel the origin of the recently found superlattice peaks in the trilayer nickelate La$_4$Ni$_3$O$_8$. These peaks arise from static charge ordering of Ni$^{2+}$/ Ni$^{1+}$ stripes oriented at 45$^{circ}$ to the Ni-O bonds. An insulating state originates from a combination of structural distortions and magnetic order, with the gap being formed solely within the d$_{x^2-y^2}$ manifold of states. When doped, electrons or holes would go into these states, in a similar fashion to what occurs in the cuprates. Analogous calculations suggest that checkerboard charge order should occur in the bilayer nickelate La$_3$Ni$_2$O$_6$. These results reveal a close connection between La$_4$Ni$_3$O$_8$ and La$_3$Ni$_2$O$_6$ with La$_{2-x}$Sr$_x$NiO$_4$ for x=1/3 and x=1/2, respectively.
We investigate the low temperature structural and physical properties of the trilayer nickelates R4Ni3O10 (R = La, Pr and Nd) using resistivity, thermopower, thermal conductivity, specific heat, high-resolution synchrotron powder X-ray diffraction and thermal expansion experiments. We show that all three compounds crystallize with a monoclinic symmetry, and undergo a metal-to-metal (MMT) transition at 135 K (La), 156 K (Pr) and 160 K (Nd). At MMT, the lattice parameters show distinct anomalies; however, without any lowering of the lattice symmetry. Unambiguous signatures of MMT are also seen in magnetic and thermal measurements, which suggest a strong coupling between the electronic, magnetic and structural degrees of freedom in these nickelates. Analysis of thermal expansion yields hydrostatic pressure dependence of MMT in close agreement with experiments. We show that the 9-fold coordinated Pr ions in the rocksalt (RS) layers have a crystal field (CF) split doublet ground state with possible antiferromagnetic ordering at 5 K. The Pr ions located in the perovskite block (PB) layers with 12-fold coordination, however, exhibit a non-magnetic singlet ground state. The CF ground state of Nd in both RS and PB layers is a Kramers doublet. Heat capacity of R = Nd shows a Schottky-like anomaly near35 K, and an upturn below T = 10 K suggesting the presence of short-range correlations between the Nd moments. However, no signs of long-range ordering could be found down to 2 K despite a sizeable theta_p ~ -40 K. The strongly suppressed magnetic long-range ordering in both R = Pr and Nd suggests the presence of strong magnetic frustration in these compounds. The low-temperature resistivity shows a T^0.5 dependence. No evidence for the heavy fermion behavior could be found in any of the three compounds.
Electronic structure calculations for spinel vanadate ZnV$_2$O$_4$ show that partial electronic delocalization in this system leads to structural instabilities. These are a consequence of the proximity to the itinerant-electron boundary, not being related to orbital ordering. We discuss how this mechanism naturally couples charge and lattice degrees of freedom in magnetic insulators close to such a crossover. For the case of ZnV$_2$O$_4$, this leads to the formation of V-V dimers along the [011] and [101] directions that readily accounts for the intriguing magnetic structure of ZnV$_2$O$_4$.
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