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1.
Proc Natl Acad Sci U S A ; 114(50): 13148-13153, 2017 12 12.
Artigo em Inglês | MEDLINE | ID: mdl-29183974

RESUMO

The value of the upper critical field Hc2, a fundamental characteristic of the superconducting state, has been subject to strong controversy in high-Tc copper oxides. Since the issue has been tackled almost exclusively by macroscopic techniques so far, there is a clear need for local-probe measurements. Here, we use 17O NMR to measure the spin susceptibility [Formula: see text] of the CuO2 planes at low temperature in charge-ordered YBa2Cu3O y We find that [Formula: see text] increases (most likely linearly) with magnetic field H and saturates above field values ranging from 20 T to 40 T. This result is consistent with the lowest Hc2 values claimed previously and with the interpretation that the charge density wave (CDW) reduces Hc2 in underdoped YBa2Cu3O y Furthermore, the absence of marked deviation in [Formula: see text] at the onset of long-range CDW order indicates that this [Formula: see text] reduction and the Fermi-surface reconstruction are primarily rooted in the short-range CDW order already present in zero field, not in the field-induced long-range CDW order. Above [Formula: see text], the relatively low values of [Formula: see text] at [Formula: see text] K show that the pseudogap is a ground-state property, independent of the superconducting gap.

2.
Inorg Chem ; 52(1): 258-72, 2013 Jan 07.
Artigo em Inglês | MEDLINE | ID: mdl-23214942

RESUMO

The synthesis and properties are reported of a rare example of a Mn(12) single-molecule magnet (SMM) in truly axial symmetry (tetragonal, I4). [Mn(12)O(12)(O(2)CCH(2)Bu(t))(16)(MeOH)(4)]·MeOH (3·MeOH) was synthesized by carboxylate substitution on [Mn(12)O(12)(O(2)CMe)(16)(H(2)O)(4)]·2MeCO(2)H·4H(2)O (1). The complex was found to possess an S = 10 ground state, as is typical for the Mn(12) family, and displayed both frequency-dependent out-of-phase AC susceptibility signals and hysteresis loops in single-crystal magnetization vs DC field sweeps. The loops also exhibited quantum tunneling of magnetization steps at periodic field values. Single-crystal, high-frequency electron paramagnetic resonance spectra on 3·MeOH using frequencies up to 360 GHz revealed perceptibly sharper signals than for 1. Moreover, careful studies as a function of the magnetic field orientation did not reveal any satellite peaks, as observed for 1, suggesting that the crystals of 3 are homogeneous and do not contain multiple Mn(12) environments. In the single-crystal (55)Mn NMR spectrum in zero applied field, three well-resolved peaks were observed, which yielded hyperfine and quadrupole splitting at three distinct sites. However, observation of a slight asymmetry in the Mn(4+) peak was detectable, suggesting a possible decrease in the local symmetry of the Mn(4+) site. Spin-lattice (T(1)) relaxation studies were performed on single crystals of 3·MeOH down to 400 mK in an effort to approach the quantum tunneling regime, and fitting of the data using multiple functions was employed. The present work and other recent studies continue to emphasize that the new generation of truly high-symmetry Mn(12) complexes are better models for thorough investigation of the physical properties of SMMs than their predecessors such as 1.

3.
Phys Rev Lett ; 105(13): 137002, 2010 Sep 24.
Artigo em Inglês | MEDLINE | ID: mdl-21230801

RESUMO

We report the results of the Knight shift by 6³,65Cu-NMR measurements on single-layered copper-oxide Bi2Sr(2-x)La(x)CuO(6+δ) conducted under very high magnetic fields up to 44 T. The magnetic field suppresses superconductivity completely, and the pseudogap ground state is revealed. The 6³Cu-NMR Knight shift shows that there remains a finite density of states at the Fermi level in the zero-temperature limit, which indicates that the pseudogap ground state is a metallic state with a finite volume of Fermi surface. The residual density of states in the pseudogap ground state decreases with decreasing doping (increasing x) but remains quite large even at the vicinity of the magnetically ordered phase of x ≥ 0.8, which suggests that the density of states plunges to zero upon approaching the Mott insulating phase.


Assuntos
Cobre/química , Condutividade Elétrica , Espectroscopia de Ressonância Magnética , Magnetismo , Cristalização
4.
Sci Rep ; 10(1): 15862, 2020 Sep 28.
Artigo em Inglês | MEDLINE | ID: mdl-32985519

RESUMO

Although the frustrated (zigzag) spin chain is the Drosophila of frustrated magnetism, our understanding of a pair of coupled zigzag chains (frustrated spin ladder) in a magnetic field is still lacking. We address this problem through nuclear magnetic resonance (NMR) experiments on BiCu[Formula: see text]PO[Formula: see text] in magnetic fields up to 45 T, revealing a field-induced spiral magnetic structure. Conjointly, we present advanced numerical calculations showing that even a moderate rung coupling dramatically simplifies the phase diagram below half-saturation magnetization by stabilizing a field-induced chiral phase. Surprisingly for a one-dimensional model, this phase and its response to Dzyaloshinskii-Moriya (DM) interactions adhere to classical expectations. While explaining the behavior at the highest accessible magnetic fields, our results imply a different origin for the solitonic phases occurring at lower fields in BiCu[Formula: see text]PO[Formula: see text]. An exciting possibility is that the known, DM-mediated coupling between chirality and crystal lattice may give rise to a new kind of spin-Peierls instability.

6.
Nat Commun ; 4: 2113, 2013.
Artigo em Inglês | MEDLINE | ID: mdl-23820931

RESUMO

Evidence is mounting that charge order competes with superconductivity in high Tc cuprates. Whether this has any relationship to the pairing mechanism is unknown as neither the universality of the competition nor its microscopic nature has been established. Here, we show using nuclear magnetic resonance that charge order in YBa2Cu3Oy has maximum strength inside the superconducting dome, similar to compounds of the La2-x(Sr,Ba)xCuO4 family. In YBa2Cu3Oy, this occurs at doping levels of p=0.11-0.12. We further show that the overlap of halos of incipient charge order around vortex cores, similar to those visualised in Bi2Sr2CaCu2O8+δ, can explain the threshold magnetic field at which long-range charge order emerges. These results reveal universal features of a competition in which charge order and superconductivity appear as joint instabilities of the same normal state, whose relative balance can be field-tuned in the vortex state.

7.
J Am Chem Soc ; 128(21): 6975-89, 2006 May 31.
Artigo em Inglês | MEDLINE | ID: mdl-16719478

RESUMO

Detailed studies are reported of a Mn(12) single-molecule magnet (SMM) in truly axial (tetragonal) symmetry. The complex is [Mn(12)O(12)(O(2)CCH(2)Br)(16)(H(2)O)(4)].4CH(2)Cl(2) (2.4CH(2)Cl(2) or Mn(12)-BrAc), obtained by the standard carboxylate substitution method. The complex has an S = 10 ground state, typical of the Mn(12) family, and displays frequency-dependent out-of-phase AC susceptibility signals and hysteresis in single-crystal magnetization vs applied DC field sweeps. Single-crystal high-frequency EPR spectra in frequencies up to 360 GHz exhibit narrow signals that are not overlapping multiplets, in contrast to [Mn(12)O(12)(O(2)CMe)(16)(H(2)O)(4)].2MeCO(2)H.4H(2)O (1 or Mn(12)-Ac), which also crystallizes in an axial (tetragonal) space group but which now is recognized to consist of a mixture of six hydrogen-bonded isomers in the crystal and thus gives multiple, inhomogeneously broadened EPR signals. Similarly, single-crystal (55)Mn NMR spectra on Mn(12)-BrAc display much sharper signals than a single crystal of Mn(12)-Ac, and this allows one Mn(III) signal to show an almost baseline-resolved quintet from quadrupolar splitting ((55)Mn, I = 5/2, 100%), allowing quadrupole coupling parameters (e(2)qQ) to be determined. In addition, it was found that crushing crystals of Mn(12)-BrAc into a microcrystalline powder causes severe broadening and shifts of the NMR resonances, emphasizing the superiority of single-crystal studies. The combined results establish that Mn(12)-BrAc is far superior to Mn(12)-Ac for the study of the intrinsic properties of the Mn(12) family of SMMs in axial symmetry, and for the search for new phenomena such as quantum interference effects caused by higher-order (>2nd-order) transverse terms in the spin Hamiltonian.

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