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1.
Proc Natl Acad Sci U S A ; 119(15): e2119429119, 2022 04 12.
Artigo em Inglês | MEDLINE | ID: mdl-35377791

RESUMO

Charge density waves (CDWs) have been observed in nearly all families of copper-oxide superconductors. But the behavior of these phases across different families has been perplexing. In La-based cuprates, the CDW wavevector is an increasing function of doping, exhibiting the so-called Yamada behavior, while in Y- and Bi-based materials the behavior is the opposite. Here, we report a combined resonant soft X-ray scattering (RSXS) and neutron scattering study of charge and spin density waves in isotopically enriched La1.8−xEu0.2SrxCuO4 over a range of doping 0.07≤x≤0.20. We find that the CDW amplitude is temperature independent and develops well above experimentally accessible temperatures. Further, the CDW wavevector shows a nonmonotonic temperature dependence, exhibiting Yamada behavior at low temperature with a sudden change occurring near the spin ordering temperature. We describe these observations using a Landau­Ginzburg theory for an incommensurate CDW in a metallic system with a finite charge compressibility and spin-CDW coupling. Extrapolating to high temperature, where the CDW amplitude is small and spin order is absent, our analysis predicts a decreasing wavevector with doping, similar to Y and Bi cuprates. Our study suggests that CDW order in all families of cuprates forms by a common mechanism.

2.
Nat Commun ; 11(1): 6167, 2020 Dec 02.
Artigo em Inglês | MEDLINE | ID: mdl-33268778

RESUMO

Thermoelectrics are promising by directly generating electricity from waste heat. However, (sub-)room-temperature thermoelectrics have been a long-standing challenge due to vanishing electronic entropy at low temperatures. Topological materials offer a new avenue for energy harvesting applications. Recent theories predicted that topological semimetals at the quantum limit can lead to a large, non-saturating thermopower and a quantized thermoelectric Hall conductivity approaching a universal value. Here, we experimentally demonstrate the non-saturating thermopower and quantized thermoelectric Hall effect in the topological Weyl semimetal (WSM) tantalum phosphide (TaP). An ultrahigh longitudinal thermopower [Formula: see text] and giant power factor [Formula: see text] are observed at ~40 K, which is largely attributed to the quantized thermoelectric Hall effect. Our work highlights the unique quantized thermoelectric Hall effect realized in a WSM toward low-temperature energy harvesting applications.

3.
Phys Rev Lett ; 124(23): 236401, 2020 Jun 12.
Artigo em Inglês | MEDLINE | ID: mdl-32603171

RESUMO

The electron-phonon interaction (EPI) is instrumental in a wide variety of phenomena in solid-state physics, such as electrical resistivity in metals, carrier mobility, optical transition, and polaron effects in semiconductors, lifetime of hot carriers, transition temperature in BCS superconductors, and even spin relaxation in diamond nitrogen-vacancy centers for quantum information processing. However, due to the weak EPI strength, most phenomena have focused on electronic properties rather than on phonon properties. One prominent exception is the Kohn anomaly, where phonon softening can emerge when the phonon wave vector nests the Fermi surface of metals. Here we report a new class of Kohn anomaly in a topological Weyl semimetal (WSM), predicted by field-theoretical calculations, and experimentally observed through inelastic x-ray and neutron scattering on WSM tantalum phosphide. Compared to the conventional Kohn anomaly, the Fermi surface in a WSM exhibits multiple topological singularities of Weyl nodes, leading to a distinct nesting condition with chiral selection, a power-law divergence, and non-negligible dynamical effects. Our work brings the concept of the Kohn anomaly into WSMs and sheds light on elucidating the EPI mechanism in emergent topological materials.

4.
Phys Rev Lett ; 124(14): 145901, 2020 Apr 10.
Artigo em Inglês | MEDLINE | ID: mdl-32338961

RESUMO

Pronounced anomalies in the SrTiO_{3} dynamical structure factor, S(Q,E), including the disappearance of acoustic phonon branches at low temperatures, were uncovered with inelastic neutron scattering (INS) and simulations. The striking effect reflects anharmonic couplings between acoustic and optic phonons and the incipient ferroelectric instability near the quantum critical point. It is rationalized using a first-principles renormalized anharmonic phonon approach, pointing to nonlinear Ti-O hybridization causing unusual changes in real-space phonon eigenvectors, frequencies, group velocities, and scattering phase space. Our method is general and establishes how T dependences beyond the harmonic regime, assessed by INS mapping of large reciprocal-space volumes, provide real-space insights into anharmonic atomic dynamics near phase transitions.

5.
Phys Rev B ; 101(14)2020.
Artigo em Inglês | MEDLINE | ID: mdl-33655092

RESUMO

We use inelastic neutron scattering to study the effect of a magnetic field on the neutron spin resonance (E r = 3.6 meV) of superconducting FeSe (T c = 9 K). While a field aligned along the in-plane direction broadens and suppresses the resonance, a c-axis aligned field does so much more efficiently, consistent with the anisotropic field-induced suppression of the superfluid density from the heat capacity measurements. These results suggest that the resonance in FeSe is associated with the superconducting electrons arising from orbital selective quasiparticle excitations between the hole and electron Fermi surfaces.

6.
Nat Commun ; 9(1): 3128, 2018 08 07.
Artigo em Inglês | MEDLINE | ID: mdl-30087342

RESUMO

Understanding the interplay between nematicity, magnetism and superconductivity is pivotal for elucidating the physics of iron-based superconductors. Here we use neutron scattering to probe magnetic and nematic orders throughout the phase diagram of NaFe1-xNixAs, finding that while both static antiferromagnetic and nematic orders compete with superconductivity, the onset temperatures for these two orders remain well separated approaching the putative quantum critical points. We uncover local orthorhombic distortions that persist well above the tetragonal-to-orthorhombic structural transition temperature Ts in underdoped samples and extend well into the overdoped regime that exhibits neither magnetic nor structural phase transitions. These unexpected local orthorhombic distortions display Curie-Weiss temperature dependence and become suppressed below the superconducting transition temperature Tc, suggesting that they result from the large nematic susceptibility near optimal superconductivity. Our results account for observations of rotational symmetry breaking above Ts, and attest to the presence of significant nematic fluctuations near optimal superconductivity.

7.
Nat Commun ; 9(1): 15, 2018 01 02.
Artigo em Inglês | MEDLINE | ID: mdl-29295988

RESUMO

Magnetoelectrics offer tantalizing opportunities for devices coupling ferroelectricity and magnetism but remain difficult to realize. Breakthrough strategies could circumvent the mutually exclusive origins of magnetism and ferroelectricity by exploiting the interaction of multiple phonon modes in geometric improper and hybrid improper ferroelectrics. Yet, the proposed instability of a zone-boundary phonon mode, driving the emergence of ferroelectricity via coupling to a polar mode, remains to be directly observed. Here, we provide previously missing evidence for this scenario in the archetypal improper ferroelectric, yttrium manganite, through comprehensive scattering measurements of the atomic structure and phonons, supported with first-principles simulations. Our experiments and theoretical modeling resolve the origin of the unusual temperature dependence of the polarization and rule out a reported double-step ferroelectric transition. These results emphasize the critical role of phonon anharmonicity in rationalizing lattice instabilities in improper ferroelectrics and show that including these effects in simulations could facilitate the design of magnetoelectrics.

8.
Nat Commun ; 7: 13879, 2016 12 19.
Artigo em Inglês | MEDLINE | ID: mdl-27991514

RESUMO

Iron-based superconductivity develops near an antiferromagnetic order and out of a bad-metal normal state, which has been interpreted as originating from a proximate Mott transition. Whether an actual Mott insulator can be realized in the phase diagram of the iron pnictides remains an open question. Here we use transport, transmission electron microscopy, X-ray absorption spectroscopy, resonant inelastic X-ray scattering and neutron scattering to demonstrate that NaFe1-xCuxAs near x≈0.5 exhibits real space Fe and Cu ordering, and are antiferromagnetic insulators with the insulating behaviour persisting above the Néel temperature, indicative of a Mott insulator. On decreasing x from 0.5, the antiferromagnetic-ordered moment continuously decreases, yielding to superconductivity ∼x=0.05. Our discovery of a Mott-insulating state in NaFe1-xCuxAs thus makes it the only known Fe-based material, in which superconductivity can be smoothly connected to the Mott-insulating state, highlighting the important role of electron correlations in the high-Tc superconductivity.

9.
Phys Rev Lett ; 117(4): 047003, 2016 Jul 22.
Artigo em Inglês | MEDLINE | ID: mdl-27494496

RESUMO

The pressure effects on the antiferromagentic orders in iron-based ladder compounds CsFe_{2}Se_{3} and BaFe_{2}S_{3} have been studied using neutron diffraction. With identical crystal structure and similar magnetic structures, the two compounds exhibit highly contrasting magnetic behaviors under moderate external pressures. In CsFe_{2}Se_{3} the ladders are brought much closer to each other by pressure, but the stripe-type magnetic order shows no observable change. In contrast, the stripe order in BaFe_{2}S_{3} undergoes a quantum phase transition where an abrupt increase of Néel temperature by more than 50% occurs at about 1 GPa, accompanied by a jump in the ordered moment. With its spin structure unchanged, BaFe_{2}S_{3} enters an enhanced magnetic phase that bears the characteristics of an orbital selective Mott phase, which is the true neighbor of superconductivity emerging at higher pressures.

10.
Phys Rev Lett ; 116(19): 197004, 2016 May 13.
Artigo em Inglês | MEDLINE | ID: mdl-27232038

RESUMO

An essential step toward elucidating the mechanism of superconductivity is to determine the sign or phase of the superconducting order parameter, as it is closely related to the pairing interaction. In conventional superconductors, the electron-phonon interaction induces attraction between electrons near the Fermi energy and results in a sign-preserved s-wave pairing. For high-temperature superconductors, including cuprates and iron-based superconductors, prevalent weak coupling theories suggest that the electron pairing is mediated by spin fluctuations which lead to repulsive interactions, and therefore that a sign-reversed pairing with an s_{±} or d-wave symmetry is favored. Here, by using magnetic neutron scattering, a phase sensitive probe of the superconducting gap, we report the observation of a transition from the sign-reversed to sign-preserved Cooper-pairing symmetry with insignificant changes in T_{c} in the S-doped iron selenide superconductors K_{x}Fe_{2-y}(Se_{1-z}S_{z})_{2}. We show that a rather sharp magnetic resonant mode well below the superconducting gap (2Δ) in the undoped sample (z=0) is replaced by a broad hump structure above 2Δ under 50% S doping. These results cannot be readily explained by simple spin fluctuation-exchange pairing theories and, therefore, multiple pairing channels are required to describe superconductivity in this system. Our findings may also yield a simple explanation for the sometimes contradictory data on the sign of the superconducting order parameter in iron-based materials.

11.
Phys Rev Lett ; 114(5): 057001, 2015 Feb 06.
Artigo em Inglês | MEDLINE | ID: mdl-25699463

RESUMO

Inelastic neutron scattering is employed to investigate the impact of electronic nematic order on the magnetic spectra of LaFeAsO and Ba(Fe(0.953)Co(0.047))(2)As(2). These materials are ideal to study the paramagnetic-nematic state, since the nematic order, signaled by the tetragonal-to-orthorhombic transition at T(S), sets in well above the stripe antiferromagnetic ordering at T(N). We find that the temperature-dependent dynamic susceptibility displays an anomaly at T(S) followed by a sharp enhancement in the spin-spin correlation length, revealing a strong feedback effect of nematic order on the low-energy magnetic spectrum. Our findings can be consistently described by a model that attributes the structural or nematic transition to magnetic fluctuations, and unveils the key role played by nematic order in promoting the long-range stripe antiferromagnetic order in iron pnictides.

12.
Phys Rev Lett ; 113(17): 177002, 2014 Oct 24.
Artigo em Inglês | MEDLINE | ID: mdl-25379931

RESUMO

The role of antiferromagnetic spin correlations in high-temperature superconductors remains a matter of debate. We present inelastic neutron-scattering evidence that gapless spin fluctuations coexist with superconductivity in La1.905Ba0.095CuO4. Furthermore, we observe that both the low-energy magnetic spectral weight and the spin incommensurability are enhanced with the onset of superconducting correlations. We propose that the coexistence occurs through intertwining of spatial modulations of the pair wave function and the antiferromagnetic correlations. This proposal is also directly relevant to sufficiently underdoped La(2-x)Sr(x)CuO(4) and YBa(2)Cu(3)O(6+x).

13.
J Phys Chem B ; 118(47): 13453-7, 2014 Nov 26.
Artigo em Inglês | MEDLINE | ID: mdl-25157644

RESUMO

Neutron diffraction patterns for deuterated poly-N,N,-dimethylacrylamide (PDMAA) hydrogels were measured from 10 to 300 K to investigate the structure and properties of water in the gels. Diffraction peaks observed below 250 K indicate the existence of ice in the hydrogels. Some diffraction peaks from the ice are at lower diffraction angles than those in ordinary hexagonal ice (Ih). These shifts in peaks indicate that the lattice constants of the a and c axes in the ice are about 0.29 and 0.3% higher than those in ice Ih, respectively. The results show that bulk low-density ice can exist in PDMAA hydrogels. The distortions in the lattice structure of ice imply significant interactions between water molecules and the surrounding polymer chains, which play an important role in the chemical and mechanical properties of the hydrogel.

14.
Nat Commun ; 5: 3467, 2014 Mar 17.
Artigo em Inglês | MEDLINE | ID: mdl-24632780

RESUMO

The insulator-to-metal transition continues to be a challenging subject, especially when electronic correlations are strong. In layered compounds, such as La2-xSrxNiO4 and La2-xBaxCuO4, the doped charge carriers can segregate into periodically spaced charge stripes separating narrow domains of antiferromagnetic order. Although there have been theoretical proposals of dynamically fluctuating stripes, direct spectroscopic evidence of charge-stripe fluctuations has been lacking. Here we report the detection of critical lattice fluctuations, driven by charge-stripe correlations, in La2-xSrxNiO4 using inelastic neutron scattering. This scattering is detected at large momentum transfers where the magnetic form factor suppresses the spin fluctuation signal. The lattice fluctuations associated with the dynamic charge stripes are narrow in q and broad in energy. They are strongest near the charge-stripe melting temperature. Our results open the way towards the quantitative theory of dynamic stripes and for directly detecting dynamical charge stripes in other strongly correlated systems, including high-temperature superconductors such as La2-xSrxCuO4.

15.
Proc Natl Acad Sci U S A ; 111(5): 1754-9, 2014 Feb 04.
Artigo em Inglês | MEDLINE | ID: mdl-24449912

RESUMO

PbZr(1-x)Ti(x)O3 (PZT) and Pb(Mg1/3Nb2/3)(1-x)Ti(x)O3 (PMN-xPT) are complex lead-oxide perovskites that display exceptional piezoelectric properties for pseudorhombohedral compositions near a tetragonal phase boundary. In PZT these compositions are ferroelectrics, but in PMN-xPT they are relaxors because the dielectric permittivity is frequency dependent and exhibits non-Arrhenius behavior. We show that the nanoscale structure unique to PMN-xPT and other lead-oxide perovskite relaxors is absent in PZT and correlates with a greater than 100% enhancement of the longitudinal piezoelectric coefficient in PMN-xPT relative to that in PZT. By comparing dielectric, structural, lattice dynamical, and piezoelectric measurements on PZT and PMN-xPT, two nearly identical compounds that represent weak and strong random electric field limits, we show that quenched (static) random fields establish the relaxor phase and identify the order parameter.

16.
Phys Rev Lett ; 107(20): 207202, 2011 Nov 11.
Artigo em Inglês | MEDLINE | ID: mdl-22181763

RESUMO

We report an inelastic neutron scattering study of acoustic phonons in the charge and orbitally ordered bilayer manganite LaSr(2)Mn(2)O(7). For excitation energies less than 15 meV, we observe an abrupt increase (decrease) of the phonon energies (linewidths) of a transverse acoustic phonon branch at q = (h, h, 0), h ≤ 0.3, upon entering the low temperature charge and orbital ordered state (T(COO) = 225 K). This indicates a reduced electron-phonon coupling due to a decrease of electronic states at the Fermi level leading to a partial removal of the Fermi surface below T(COO) and provides direct experimental evidence for a link between electron-phonon coupling and charge order in manganites.

17.
Sci Rep ; 1: 115, 2011.
Artigo em Inglês | MEDLINE | ID: mdl-22355632

RESUMO

We report inelastic neutron scattering experiments on single crystals of superconducting Ba(0.67)K(0.33)Fe(2)As(2) (T(c) = 38 K). In addition to confirming the resonance previously found in powder samples, we find that spin excitations in the normal state form longitudinally elongated ellipses along the Q(AFM) direction in momentum space, consistent with density functional theory predictions. On cooling below T(c), while the resonance preserves its momentum anisotropy as expected, spin excitations at energies below the resonance become essentially isotropic in the in-plane momentum space and dramatically increase their correlation length. These results suggest that the superconducting gap structures in Ba(0.67)Ka(0.33)Fe(2)As(2) are more complicated than those suggested from angle resolved photoemission experiments.

18.
Phys Rev Lett ; 103(16): 167202, 2009 Oct 16.
Artigo em Inglês | MEDLINE | ID: mdl-19905720

RESUMO

We use neutron scattering to investigate the doping evolution of the magnetic correlations in the single-layer manganite Pr1-xCa1+xMnO4, away from the x=0.5 composition where the CE-type commensurate antiferromagnetic (AF) structure is stable. We find that short-range incommensurate spin correlations develop as the system is electron doped (x<0.5), which coexist with the CE-type AF order. This suggests that electron doping in this system induces an inhomogeneous electronic self-organization, where commensurate AF patches with x=0.5 are separated by electron-rich domain walls with short-range magnetic correlations. This behavior is strikingly different than for the perovskite Pr1-xCaxMnO3, where the long-range CE-type commensurate AF structure is stable over a wide range of electron or hole doping around x=0.5.

19.
Phys Rev Lett ; 102(10): 107006, 2009 Mar 13.
Artigo em Inglês | MEDLINE | ID: mdl-19392150

RESUMO

We use inelastic neutron scattering to study magnetic excitations of the FeAs-based superconductor BaFe1.9Ni0.1As2 above and below its T_{c} (=20 K). In addition to gradually open a spin gap at the in-plane antiferromagnetic ordering wave vector (1, 0, 0), the effect of superconductivity is to form a three-dimensional resonance with clear dispersion along the c axis. The intensity of the resonance develops like a superconducting order parameter, and the mode occurs at distinctively different energies at (1, 0, 0) and (1, 0, 1). If the resonance energy is associated with the superconducting gap energy Delta, then Delta is dependent on the wave vector transfers along the c axis. These results suggest that one must be careful in interpreting the superconducting gap energies obtained by surface sensitive probes such as scanning tunneling microscopy and angle resolved photoemission.

20.
Phys Rev Lett ; 101(21): 217002, 2008 Nov 21.
Artigo em Inglês | MEDLINE | ID: mdl-19113445

RESUMO

We use inelastic neutron scattering to study the crystalline electric field (CEF) excitations of Ce3+ in CeFeAsO(1-x)F(x) (x=0, 0.16). For nonsuperconducting CeFeAsO, the Ce CEF levels have three magnetic doublets in the paramagnetic state, but these doublets split into six singlets when the Fe ions order antiferromagnetically. For superconducting CeFeAsO0.84F0.16 T(c)=41 K), where the static antiferromagnetic order is suppressed, the Ce CEF levels have three magnetic doublets at [formula: see text], 18.7, 58.4 meV at all temperatures. Careful measurements of the intrinsic linewidth Gamma and the peak position of the 18.7 meV mode reveal a clear anomaly at T(c), consistent with a strong enhancement of local magnetic susceptibility chi'' [formula: see text] below T(c). These results suggest that CEF excitations in the rare-earth oxypnictides can be used as a probe of spin dynamics in the nearby FeAs planes.

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