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1.
Proc Natl Acad Sci U S A ; 118(51)2021 Dec 21.
Artigo em Inglês | MEDLINE | ID: mdl-34911757

RESUMO

Magnetoelastic dilatometry of the piezomagnetic antiferromagnet UO2 was performed via the fiber Bragg grating method in magnetic fields up to 150 T generated by a single-turn coil setup. We show that in microsecond timescales, pulsed-magnetic fields excite mechanical resonances at temperatures ranging from 10 to 300 K, in the paramagnetic as well as within the robust antiferromagnetic state of the material. These resonances, which are barely attenuated within the 100-µs observation window, are attributed to the strong magnetoelastic coupling in UO2 combined with the high crystalline quality of the single crystal samples. They compare well with mechanical resonances obtained by a resonant ultrasound technique and superimpose on the known nonmonotonic magnetostriction background. A clear phase shift of π in the lattice oscillations is observed in the antiferromagnetic state when the magnetic field overcomes the piezomagnetic switch field H[Formula: see text] T. We present a theoretical argument that explains this unexpected behavior as a result of the reversal of the antiferromagnetic order parameter at Hc.

2.
Proc Natl Acad Sci U S A ; 117(18): 9782-9786, 2020 May 05.
Artigo em Inglês | MEDLINE | ID: mdl-32317380

RESUMO

High magnetic fields have revealed a surprisingly small Fermi surface in underdoped cuprates, possibly resulting from Fermi-surface reconstruction due to an order parameter that breaks translational symmetry of the crystal lattice. A crucial issue concerns the doping extent of such a state and its relationship to the principal pseudogap and superconducting phases. We employ pulsed magnetic-field measurements on the cuprate [Formula: see text]Cu[Formula: see text] to identify signatures of Fermi-surface reconstruction from a sign change of the Hall effect and a peak in the temperature-dependent planar resistivity. We trace the termination of Fermi-surface reconstruction to two hole concentrations where the superconducting upper critical fields are found to be enhanced. One of these points is associated with the pseudogap endpoint near optimal doping. These results connect the Fermi-surface reconstruction to both superconductivity and the pseudogap phenomena.

3.
Nat Mater ; 19(2): 163-169, 2020 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-31819211

RESUMO

A kagome lattice of 3d transition metal ions is a versatile platform for correlated topological phases hosting symmetry-protected electronic excitations and magnetic ground states. However, the paradigmatic states of the idealized two-dimensional kagome lattice-Dirac fermions and flat bands-have not been simultaneously observed. Here, we use angle-resolved photoemission spectroscopy and de Haas-van Alphen quantum oscillations to reveal coexisting surface and bulk Dirac fermions as well as flat bands in the antiferromagnetic kagome metal FeSn, which has spatially decoupled kagome planes. Our band structure calculations and matrix element simulations demonstrate that the bulk Dirac bands arise from in-plane localized Fe-3d orbitals, and evidence that the coexisting Dirac surface state realizes a rare example of fully spin-polarized two-dimensional Dirac fermions due to spin-layer locking in FeSn. The prospect to harness these prototypical excitations in a kagome lattice is a frontier of great promise at the confluence of topology, magnetism and strongly correlated physics.

4.
Nature ; 498(7452): 75-7, 2013 Jun 06.
Artigo em Inglês | MEDLINE | ID: mdl-23739425

RESUMO

Close to optimal doping, the copper oxide superconductors show 'strange metal' behaviour, suggestive of strong fluctuations associated with a quantum critical point. Such a critical point requires a line of classical phase transitions terminating at zero temperature near optimal doping inside the superconducting 'dome'. The underdoped region of the temperature-doping phase diagram from which superconductivity emerges is referred to as the 'pseudogap' because evidence exists for partial gapping of the conduction electrons, but so far there is no compelling thermodynamic evidence as to whether the pseudogap is a distinct phase or a continuous evolution of physical properties on cooling. Here we report that the pseudogap in YBa2Cu3O6+δ is a distinct phase, bounded by a line of phase transitions. The doping dependence of this line is such that it terminates at zero temperature inside the superconducting dome. From this we conclude that quantum criticality drives the strange metallic behaviour and therefore superconductivity in the copper oxide superconductors.

5.
Phys Rev Lett ; 121(19): 197002, 2018 Nov 09.
Artigo em Inglês | MEDLINE | ID: mdl-30468585

RESUMO

The phenomenon of T-linear resistivity commonly observed in a number of strange metals has been widely seen as evidence for the breakdown of the quasiparticle picture of metals. This study shows that a recently discovered H/T scaling relationship in the magnetoresistance of the strange metal BaFe_{2}(As_{1-x}P_{x})_{2} is independent of the relative orientations of current and magnetic field. Rather, its magnitude and form depend only on the orientation of the magnetic field with respect to a single crystallographic axis: the direction perpendicular to the magnetic iron layers. This finding suggests that the magnetotransport scaling does not originate from the conventional averaging or orbital velocity of quasiparticles as they traverse a Fermi surface, but rather from dissipation arising from two-dimensional correlations.

6.
Proc Natl Acad Sci U S A ; 112(11): 3285-9, 2015 Mar 17.
Artigo em Inglês | MEDLINE | ID: mdl-25737548

RESUMO

The d and f electrons in correlated metals are often neither fully localized around their host nuclei nor fully itinerant. This localized/itinerant duality underlies the correlated electronic states of the high-Tc cuprate superconductors and the heavy-fermion intermetallics and is nowhere more apparent than in the 5f valence electrons of plutonium. Here, we report the full set of symmetry-resolved elastic moduli of PuCoGa5--the highest Tc superconductor of the heavy fermions (Tc = 18.5 K)--and find that the bulk modulus softens anomalously over a wide range in temperature above Tc. The elastic symmetry channel in which this softening occurs is characteristic of a valence instability--therefore, we identify the elastic softening with fluctuations of the plutonium 5f mixed-valence state. These valence fluctuations disappear when the superconducting gap opens at Tc, suggesting that electrons near the Fermi surface play an essential role in the mixed-valence physics of this system and that PuCoGa5 avoids a valence transition by entering the superconducting state. The lack of magnetism in PuCoGa5 has made it difficult to reconcile with most other heavy-fermion superconductors, where superconductivity is generally believed to be mediated by magnetic fluctuations. Our observations suggest that valence fluctuations play a critical role in the unusually high Tc of PuCoGa5.

7.
PNAS Nexus ; 3(1): pgad428, 2024 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-38234583

RESUMO

There has been a recent surge of interest in UTe2 due to its unconventional magnetic field (H)-reinforced spin-triplet superconducting phases persisting at fields far above the simple Pauli limit for H∥[010]. Magnetic fields in excess of 35 T then induce a field-polarized magnetic state via a first-order-like phase transition. More controversially, for field orientations close to H∥[011] and above 40 T, electrical resistivity measurements suggest that a further superconducting state may exist. However, no Meissner effect or thermodynamic evidence exists to date for this phase making it difficult to exclude alternative scenarios. In this paper, we describe a study using thermal, electrical, and magnetic probes in magnetic fields of up to 55 T applied between the [010] (b) and [001] (c) directions. Our MHz conductivity data reveal the field-induced state of low or vanishing electrical resistance; our simultaneous magnetocaloric effect measurements (i.e. changes in sample temperature due to changing magnetic field) show the first definitive evidence for adiabaticity and thermal behavior characteristic of bulk field-induced superconductivity.

8.
Phys Rev Lett ; 109(16): 167204, 2012 Oct 19.
Artigo em Inglês | MEDLINE | ID: mdl-23215121

RESUMO

BiCu(2)PO(6) is a frustrated two-leg spin-ladder compound with a spin gap that can be closed with a magnetic field of approximately 20 T. This quantum phase transition and its related phase diagram as a function of magnetic field and temperature (H, T) are investigated up to 60 T by means of specific heat, magnetocaloric effect, magnetization, and magnetostriction measurements. In contrast to other gapped quantum magnets, BiCu(2)PO(6) undergoes a series of unexpected first- and second-order phase transitions when an external magnetic field is applied along the crystallographic c axis. The application of a magnetic field along the b axis induces two second-order phase transitions. We propose that the anisotropy and complex phase diagram result from the interplay between strong geometrical frustration and spin-orbit interaction necessary for the description of this fascinating magnetic system.

9.
Phys Rev Lett ; 108(7): 077208, 2012 Feb 17.
Artigo em Inglês | MEDLINE | ID: mdl-22401252

RESUMO

Gaining control of the building blocks of magnetic materials and thereby achieving particular characteristics will make possible the design and growth of bespoke magnetic devices. While progress in the synthesis of molecular materials, and especially coordination polymers, represents a significant step towards this goal, the ability to tune the magnetic interactions within a particular framework remains in its infancy. Here we demonstrate a chemical method which achieves dimensionality selection via preferential inhibition of the magnetic exchange in an S=1/2 antiferromagnet along one crystal direction, switching the system from being quasi-two- to quasi-one-dimensional while effectively maintaining the nearest-neighbor coupling strength.

10.
Inorg Chem ; 50(13): 5990-6009, 2011 Jul 04.
Artigo em Inglês | MEDLINE | ID: mdl-21598910

RESUMO

[Ni(HF(2))(pyz)(2)]X {pyz = pyrazine; X = PF(6)(-) (1), SbF(6)(-) (2)} were structurally characterized by synchrotron X-ray powder diffraction and found to possess axially compressed NiN(4)F(2) octahedra. At 298 K, 1 is monoclinic (C2/c) with unit cell parameters, a = 9.9481(3), b = 9.9421(3), c = 12.5953(4) Å, and ß = 81.610(3)° while 2 is tetragonal (P4/nmm) with a = b = 9.9359(3) and c = 6.4471(2) Å and is isomorphic with the Cu-analogue. Infinite one-dimensional (1D) Ni-FHF-Ni chains propagate along the c-axis which are linked via µ-pyz bridges in the ab-plane to afford three-dimensional polymeric frameworks with PF(6)(-) and SbF(6)(-) counterions occupying the interior sites. A major difference between 1 and 2 is that the Ni-F-H bonds are bent (∼157°) in 1 but are linear in 2. Ligand field calculations (LFT) based on an angular overlap model (AOM), with comparison to the electronic absorption spectra, indicate greater π-donation of the HF(2)(-) ligand in 1 owing to the bent Ni-F-H bonds. Magnetic susceptibility data for 1 and 2 exhibit broad maxima at 7.4 and 15 K, respectively, and λ-like peaks in dχT/dT at 6.2 and 12.2 K that are ascribed to transitions to long-range antiferromagnetic order (T(N)). Muon-spin relaxation and specific heat studies confirm these T(N)'s. A comparative analysis of χ vs T to various 1D Heisenberg/Ising models suggests moderate antiferromagnetic interactions, with the primary interaction strength determined to be 3.05/3.42 K (1) and 5.65/6.37 K (2). However, high critical fields of 19 and 37.4 T obtained from low temperature pulsed-field magnetization data indicate that a single exchange constant (J(1D)) alone is insufficient to explain the data and that residual terms in the spin Hamiltonian, which could include interchain magnetic couplings (J(⊥)), as mediated by Ni-pyz-Ni, and single-ion anisotropy (D), must be considered. While it is difficult to draw absolute conclusions regarding the magnitude (and sign) of J(⊥) and D based solely on powder data, further support offered by related Ni(II)-pyz compounds and our LFT and density-functional theory (DFT) results lead us to a consistent quasi-1D magnetic description for 1 and 2.


Assuntos
Elétrons , Magnetismo , Compostos Organometálicos/química , Teoria Quântica , Ácido Fluorídrico/química , Estrutura Molecular , Níquel/química , Compostos Organometálicos/síntese química , Pirazinas/química
11.
Nat Commun ; 11(1): 560, 2020 Jan 28.
Artigo em Inglês | MEDLINE | ID: mdl-31992704

RESUMO

Co[Formula: see text]Sn[Formula: see text]S[Formula: see text] is a ferromagnetic Weyl semimetal that has been the subject of intense scientific interest due to its large anomalous Hall effect. We show that the coupling of this material's topological properties to its magnetic texture leads to a strongly exchange biased anomalous Hall effect. We argue that this is likely caused by the coexistence of ferromagnetism and geometric frustration intrinsic to the kagome network of magnetic ions, giving rise to spin-glass behavior and an exchange bias.

12.
J Am Chem Soc ; 131(13): 4590-1, 2009 Apr 08.
Artigo em Inglês | MEDLINE | ID: mdl-19334770

RESUMO

X-ray powder diffraction and magnetic susceptibility measurements show that Ag(pyz)(2)(S(2)O(8)) consists of 2D square nets of Ag(2+) ions resulting from the corner-sharing of axially elongated AgN(4)O(2) octahedra and exhibits characteristic 2D antiferromagnetism. Nevertheless, mu(+)SR measurements indicate that Ag(pyz)(2)(S(2)O(8)) undergoes 3D magnetic ordering below 7.8(3) K.

13.
J Am Chem Soc ; 131(19): 6733-47, 2009 May 20.
Artigo em Inglês | MEDLINE | ID: mdl-19290599

RESUMO

Three Cu(2+)-containing coordination polymers were synthesized and characterized by experimental (X-ray diffraction, magnetic susceptibility, pulsed-field magnetization, heat capacity, and muon-spin relaxation) and electronic structure studies (quantum Monte Carlo simulations and density functional theory calculations). [Cu(HF(2))(pyz)(2)]SbF(6) (pyz = pyrazine) (1a), [Cu(2)F(HF)(HF(2))(pyz)(4)](SbF(6))(2) (1b), and [CuAg(H(3)F(4))(pyz)(5)](SbF(6))(2) (2) crystallize in either tetragonal or orthorhombic space groups; their structures consist of 2D square layers of [M(pyz)(2)](n+) that are linked in the third dimension by either HF(2)(-) (1a and 1b) or H(3)F(4)(-) (2). The resulting 3D frameworks contain charge-balancing SbF(6)(-) anions in every void. Compound 1b is a defective polymorph of 1a, with the difference being that 50% of the HF(2)(-) links are broken in the former, which leads to a cooperative Jahn-Teller distortion and d(x(2))(-y(2)) orbital ordering. Magnetic data for 1a and 1b reveal broad maxima in chi at 12.5 and 2.6 K and long-range magnetic order below 4.3 and 1.7 K, respectively, while 2 displays negligible spin interactions owing to long and disrupted superexchange pathways. The isothermal magnetization, M(B), for 1a and 1b measured at 0.5 K reveals contrasting behaviors: 1a exhibits a concave shape as B increases to a saturation field, B(c), of 37.6 T, whereas 1b presents an unusual two-step saturation in which M(B) is convex until it reaches a step near 10.8 T and then becomes concave until saturation is reached at 15.8 T. The step occurs at two-thirds of M(sat), suggesting the presence of a ferrimagnetic structure. Compound 2 shows unusual hysteresis in M(B) at low temperature, although chi vs T does not reveal the presence of a magnetic phase transition. Quantum Monte Carlo simulations based on an anisotropic cubic lattice were applied to the magnetic data of 1a to afford g = 2.14, J = -13.4 K (Cu-pyz-Cu), and J(perpendicular) = -0.20 K (Cu-F...H...F-Cu), while chi vs T for 1b could be well reproduced by a spin-1/2 Heisenberg uniform chain model for g = 2.127(1), J(1) = -3.81(1), and zJ(2) = -0.48(1) K, where J(1) and J(2) are the intra- and interchain exchange couplings, respectively, which considers the number of magnetic nearest-neighbors (z). The M(B) data for 1b could not be satisfactorily explained by the chain model, suggesting a more complex magnetic structure in the ordered state and the need for additional terms in the spin Hamiltonian. The observed variation in magnetic behaviors is driven by differences in the H...F hydrogen-bonding motifs.

14.
J Phys Condens Matter ; 21(1): 012201, 2009 Jan 07.
Artigo em Inglês | MEDLINE | ID: mdl-21817202

RESUMO

We propose that the extraordinarily high superconducting transition temperatures in the cuprates are driven by an exact mapping of the d(x(2)-y(2)) Cooper-pair wavefunction onto the incommensurate spin fluctuations observed in neutron-scattering experiments. This is manifested in the direct correspondence between the inverse of the incommensurability factor δ seen in inelastic neutron-scattering experiments and the measured superconducting coherence length ξ(0). Strikingly, the relationship between ξ(0) and δ is valid for both La(2-x)Sr(x)CuO(4) and YBa(2)Cu(3)O(7-x), suggesting a common mechanism for superconductivity across the entire hole-doped cuprate family. Using data from recent quantum-oscillation experiments in the cuprates, we propose that the fluctuations responsible for superconductivity are driven by a Fermi-surface instability. On the basis of these findings, one can specify the optimal characteristics of a solid that will exhibit 'high T(c)' superconductivity.

15.
Nat Commun ; 10(1): 4870, 2019 10 25.
Artigo em Inglês | MEDLINE | ID: mdl-31653866

RESUMO

Primarily considered a medium of geometric frustration, there has been a growing recognition of the kagome network as a harbor of lattice-borne topological electronic phases. In this study we report the observation of magnetoquantum de Haas-van Alphen oscillations of the ferromagnetic kagome lattice metal Fe3Sn2. We observe a pair of quasi-two-dimensional Fermi surfaces arising from bulk massive Dirac states and show that these band areas and effective masses are systematically modulated by the rotation of the ferromagnetic moment. Combined with measurements of Berry curvature induced Hall conductivity, our observations suggest that the ferromagnetic Dirac fermions in Fe3Sn2 are subject to intrinsic spin-orbit coupling in the d electron sector which is likely of Kane-Mele type. Our results provide insights for spintronic manipulation of magnetic topological electronic states and pathways to realizing further highly correlated topological materials from the lattice perspective.

16.
Science ; 366(6462): 221-226, 2019 10 11.
Artigo em Inglês | MEDLINE | ID: mdl-31601766

RESUMO

Although crystals of strongly correlated metals exhibit a diverse set of electronic ground states, few approaches exist for spatially modulating their properties. In this study, we demonstrate disorder-free control, on the micrometer scale, over the superconducting state in samples of the heavy-fermion superconductor CeIrIn5 We pattern crystals by focused ion beam milling to tailor the boundary conditions for the elastic deformation upon thermal contraction during cooling. The resulting nonuniform strain fields induce complex patterns of superconductivity, owing to the strong dependence of the transition temperature on the strength and direction of strain. These results showcase a generic approach to manipulating electronic order on micrometer length scales in strongly correlated matter without compromising the cleanliness, stoichiometry, or mean free path.

17.
Nat Commun ; 9(1): 3975, 2018 09 28.
Artigo em Inglês | MEDLINE | ID: mdl-30266902

RESUMO

Unusual behavior in quantum materials commonly arises from their effective low-dimensional physics, reflecting the underlying anisotropy in the spin and charge degrees of freedom. Here we introduce the magnetotropic coefficient k = ∂2F/∂θ2, the second derivative of the free energy F with respect to the magnetic field orientation θ in the crystal. We show that the magnetotropic coefficient can be quantitatively determined from a shift in the resonant frequency of a commercially available atomic force microscopy cantilever under magnetic field. This detection method enables part per 100 million sensitivity and the ability to measure magnetic anisotropy in nanogram-scale samples, as demonstrated on the Weyl semimetal NbP. Measurement of the magnetotropic coefficient in the spin-liquid candidate RuCl3 highlights its sensitivity to anisotropic phase transitions and allows a quantitative comparison to other thermodynamic coefficients via the Ehrenfest relations.

18.
Nat Commun ; 8: 15297, 2017 05 19.
Artigo em Inglês | MEDLINE | ID: mdl-28524844

RESUMO

The Fermi surface of elemental bismuth consists of three small rotationally equivalent electron pockets, offering a valley degree of freedom to charge carriers. A relatively small magnetic field can confine electrons to their lowest Landau level. This is the quantum limit attained in other dilute metals upon application of sufficiently strong magnetic field. Here we report on the observation of another threshold magnetic field never encountered before in any other solid. Above this field, Bempty, one or two valleys become totally empty. Drying up a Fermi sea by magnetic field in the Brillouin zone leads to a manyfold enhancement in electric conductance. We trace the origin of the large drop in magnetoresistance across Bempty to transfer of carriers between valleys with highly anisotropic mobilities. The non-interacting picture of electrons with field-dependent mobility explains most results but the Coulomb interaction may play a role in shaping the fine details.

19.
Nat Commun ; 8(1): 180, 2017 08 01.
Artigo em Inglês | MEDLINE | ID: mdl-28765523

RESUMO

The complex antiferromagnetic orders observed in the honeycomb iridates are a double-edged sword in the search for a quantum spin-liquid: both attesting that the magnetic interactions provide many of the necessary ingredients, while simultaneously impeding access. Focus has naturally been drawn to the unusual magnetic orders that hint at the underlying spin correlations. However, the study of any particular broken symmetry state generally provides little clue about the possibility of other nearby ground states. Here we use magnetic fields approaching 100 Tesla to reveal the extent of the spin correlations in γ-lithium iridate. We find that a small component of field along the magnetic easy-axis melts long-range order, revealing a bistable, strongly correlated spin state. Far from the usual destruction of antiferromagnetism via spin polarization, the high-field state possesses only a small fraction of the total iridium moment, without evidence for long-range order up to the highest attainable magnetic fields.The complex antiferromagnetic orders observed in the honeycomb iridates prevent access to a spin-liquid ground state. Here the authors apply extremely high magnetic fields to destroy the antiferromagnetic order in γ-lithium iridate and reveal a bistable, strongly correlated spin state.

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