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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.
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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.
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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.
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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.
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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.
RESUMEN
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.
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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.
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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).
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Ferroic materials on the verge of forming ferroic glasses exhibit heightened functionality that is often attributed to competing long- and short-range correlations. However, the physics underlying these enhancements is not well understood. The Ni45Co5Mn36.6In13.4 Heusler alloy is on the edge of forming both spin and strain glasses and exhibits magnetic field-induced shape memory and large magnetocaloric effects, making it a candidate for multicaloric cooling applications. We show using neutron scattering that localized magnon-phonon hybrid modes, which are inherently spread across reciprocal space, act as a bridge between phonons and magnons and result in substantial magnetic field-induced shifts in the phonons, triple the caloric response, and alter phase stability. We attribute these modes to the localization of phonons and magnons by antiphase boundaries coupled to magnetic domains. Because the interplay between short- and long-range correlations is common near ferroic glassy states, our work provides general insights on how glassiness enhances function.
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Stacking two-dimensional (2D) van der Waals (vdW) materials in a layered bulk structure provides an appealing platform for the emergence of exotic physical properties. As a vdW crystal with exceptional plasticity, InSe offers the opportunity to explore various effects arising from the coupling of its peculiar mechanical behaviors and other physical properties. Here, we employ neutron scattering techniques to investigate the correlations of plastic interlayer slip, lattice anharmonicity, and thermal transport in InSe crystals. Not only are the interlayer slip direction and magnitude well captured by shifts in the Bragg reflections, but we also observe a deviation from the expected Debye behaviour in the heat capacity and lattice thermal conductivity. Combining the experimental data with first-principles calculations, we tentatively attribute the observed evidence of strong phonon-phonon interactions to a combination of a large acoustic-optical frequency resonance and a nesting effect. These findings correlate the macroscopic plastic slip and the microscopic lattice dynamics, providing insights into the mechano-thermo coupling and modulation in 2D vdW materials.
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The interplay between magnetism and electronic band topology enriches topological phases and has promising applications. However, the role of topology in magnetic fluctuations has been elusive. Here, we report evidence for topology stabilized magnetism above the magnetic transition temperature in magnetic Weyl semimetal candidate CeAlGe. Electrical transport, thermal transport, resonant elastic X-ray scattering, and dilatometry consistently indicate the presence of locally correlated magnetism within a narrow temperature window well above the thermodynamic magnetic transition temperature. The wavevector of this short-range order is consistent with the nesting condition of topological Weyl nodes, suggesting that it arises from the interaction between magnetic fluctuations and the emergent Weyl fermions. Effective field theory shows that this topology stabilized order is wavevector dependent and can be stabilized when the interband Weyl fermion scattering is dominant. Our work highlights the role of electronic band topology in stabilizing magnetic order even in the classically disordered regime.
RESUMEN
In conventional superconductors, the interaction that pairs the electrons to form the superconducting state is mediated by lattice vibrations (phonons). In high-transition-temperature (high-T(c)) copper oxides, it is generally believed that magnetic excitations might play a fundamental role in the superconducting mechanism because superconductivity occurs when mobile 'electrons' or 'holes' are doped into the antiferromagnetic parent compounds. Indeed, a sharp magnetic excitation termed 'resonance' has been observed by neutron scattering in a number of hole-doped materials. The resonance is intimately related to superconductivity, and its interaction with charged quasi-particles observed by photoemission, optical conductivity, and tunnelling suggests that it might play a part similar to that of phonons in conventional superconductors. The relevance of the resonance to high-T(c) superconductivity, however, has been in doubt because so far it has been found only in hole-doped materials. Here we report the discovery of the resonance in electron-doped superconducting Pr0.88LaCe0.12CuO4-delta (T(c) = 24 K). We find that the resonance energy (E(r)) is proportional to T(c) via E(r) approximately 5.8k(B)T(c) for all high-T(c) superconductors irrespective of electron- or hole-doping. Our results demonstrate that the resonance is a fundamental property of the superconducting copper oxides and therefore must be essential in the mechanism of superconductivity.
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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.
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Geometric frustration in the kagome lattice makes it a great host for the flat electronic band, nontrivial topological properties, and novel magnetism. Here, we use magnetotransport measurements to map out the field-temperature phase diagram of the centrosymmetric YMn6Sn6 with a Mn kagome lattice and show that the system exhibits the topological Hall effect (THE) with an in-plane applied magnetic field around 240 K. In addition, our neutron diffraction results demonstrate that the observed THE cannot arise from a magnetic skyrmion lattice, but instead from an in-plane field-induced double-fan spin structure with c -axis components. This paper provides a platform to understand the influence of a field-induced novel magnetic structure on magnetoelectric response in topological kagome metals.
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We use neutron scattering to study the lattice and magnetic structure of the layered half-doped manganite Pr(0.5)Ca(1.5)MnO(4). On cooling from high temperature, the system first becomes charge-and orbital-ordered (CO/OO) near T(CO) = 300 K and then develops checkerboard-like antiferromagnetic (AF) order below T(N) = 130 K. At temperatures above T(N) but below T(CO) (T(N)
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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.
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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.
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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.
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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.
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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.