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1.
Inorg Chem ; 59(20): 15144-15153, 2020 Oct 19.
Article in English | MEDLINE | ID: mdl-33021788

ABSTRACT

In this paper, the hyperkagome lattice of Gd spins in a garnet compound, Gd3CrGa4O12, is studied using bulk measurements and density functional computations, and the observation of large magnetocaloric effect corresponding to an entropy change, ΔSm = 45 J kg-1K-1 (≈ 45 J mol-1K-1) at 2 K, 8 T is reported. Though the compound defies long-range magnetic order down to 0.4 K, a broad feature below 10 K is observed in the specific heat with two low temperature anomalies at T* ≈ 0.7 K and TS ≈ 2.45 K. The anomaly at T* is reminiscent of one in Gd3Ga5O12, where it is related to the development of a complex magnetic phase, whereas the TS-peak is accounted for by a multilevel Schottky-like model. The spin-lattice relaxation times studied by nuclear magnetic resonance experiments show that the relaxation is dominated by the magnetic fluctuations in Cr which has a longer relaxation time compared to that of the garnet, Lu3CrGa4O12 containing a nonmagnetic rare earth. Our first-principles density functional theory calculations agree well with the experimental results and support short-range magnetic order in the Gd-sublattice and antiferromagnetism in the Cr-sublattice. The importance of spin fluctuations and short-range order in the rare earth and transition metal lattices in garnets resulting in large magnetocaloric effect is brought out through this work.

2.
Nat Commun ; 9(1): 4327, 2018 10 18.
Article in English | MEDLINE | ID: mdl-30337539

ABSTRACT

A pivotal step toward understanding unconventional superconductors would be to decipher how superconductivity emerges from the unusual normal state. In the cuprates, traces of superconducting pairing appear above the macroscopic transition temperature Tc, yet extensive investigation has led to disparate conclusions. The main difficulty has been to separate superconducting contributions from complex normal-state behaviour. Here we avoid this problem by measuring nonlinear conductivity, an observable that is zero in the normal state. We uncover for several representative cuprates that the nonlinear conductivity vanishes exponentially above Tc, both with temperature and magnetic field, and exhibits temperature-scaling characterized by a universal scale Ξ0. Attempts to model the response with standard Ginzburg-Landau theory are systematically unsuccessful. Instead, our findings are captured by a simple percolation model that also explains other properties of the cuprates. We thus resolve a long-standing conundrum by showing that the superconducting precursor in the cuprates is strongly affected by intrinsic inhomogeneity.

3.
Proc Natl Acad Sci U S A ; 110(30): 12235-40, 2013 Jul 23.
Article in English | MEDLINE | ID: mdl-23836669

ABSTRACT

Upon introducing charge carriers into the copper-oxygen sheets of the enigmatic lamellar cuprates, the ground state evolves from an insulator to a superconductor and eventually to a seemingly conventional metal (a Fermi liquid). Much has remained elusive about the nature of this evolution and about the peculiar metallic state at intermediate hole-carrier concentrations (p). The planar resistivity of this unconventional metal exhibits a linear temperature dependence (ρ ∝ T) that is disrupted upon cooling toward the superconducting state by the opening of a partial gap (the pseudogap) on the Fermi surface. Here, we first demonstrate for the quintessential compound HgBa2CuO4+δ a dramatic switch from linear to purely quadratic (Fermi liquid-like, ρ ∝ T(2)) resistive behavior in the pseudogap regime. Despite the considerable variation in crystal structures and disorder among different compounds, our result together with prior work gives insight into the p-T phase diagram and reveals the fundamental resistance per copper-oxygen sheet in both linear (ρ = A1T) and quadratic (ρ = A2T(2)) regimes, with A1 ∝ A2 ∝ 1/p. Theoretical models can now be benchmarked against this remarkably simple universal behavior. Deviations from this underlying behavior can be expected to lead to new insight into the nonuniversal features exhibited by certain compounds.

4.
Proc Natl Acad Sci U S A ; 110(15): 5774-8, 2013 Apr 09.
Article in English | MEDLINE | ID: mdl-23536291

ABSTRACT

Cuprate high-Tc superconductors exhibit enigmatic behavior in the nonsuperconducting state. For carrier concentrations near "optimal doping" (with respect to the highest Tcs) the transport and spectroscopic properties are unlike those of a Landau-Fermi liquid. On the Mott-insulating side of the optimal carrier concentration, which corresponds to underdoping, a pseudogap removes quasi-particle spectral weight from parts of the Fermi surface and causes a breakup of the Fermi surface into disconnected nodal and antinodal sectors. Here, we show that the near-nodal excitations of underdoped cuprates obey Fermi liquid behavior. The lifetime τ(ω, T) of a quasi-particle depends on its energy ω as well as on the temperature T. For a Fermi liquid, 1/τ(ω, T) is expected to collapse on a universal function proportional to (ℏω)(2) + (pπk(B)T)(2). Magneto-transport experiments, which probe the properties in the limit ω = 0, have provided indications for the presence of a T(2) dependence of the dc (ω = 0) resistivity of different cuprate materials. However, Fermi liquid behavior is very much about the energy dependence of the lifetime, and this can only be addressed by spectroscopic techniques. Our optical experiments confirm the aforementioned universal ω- and T dependence of 1/τ(ω, T), with p ∼ 1.5. Our data thus provide a piece of evidence in favor of a Fermi liquid-like scenario of the pseudogap phase of the cuprates.

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