Bond ordering and molecular spin-orbital fluctuations in the cluster Mott insulator GaTa 4 Se 8
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36 MATERIALS SCIENCE↗
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Results for “spin fluctuation”
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Coupled electronic and magnetic excitations in the cuprates and their role in the superconducting transition
The formation of Cooper pairs, a bound state of two electrons of opposite spin and momenta by exchange of a phonon, is a defining feature of conventional superconductivity. In the cuprate high temperature superconductors, even though the superconducting state also consists of Cooper pairs, the pairing mechanism remains intensely debated. Here, we investigate superconducting pairing in the Bi 2 Sr 2 CaCu 2 O 8+δ (Bi2212) cuprate by employing spectral functions obtained from angle-resolved photoemission as input to the Bethe-Salpeter equation. Assuming Cooper pairing is driven by spin fluctuations, we construct the spin-fluctuation-mediated pairing interaction and use it to compute the eigenfunctions and eigenvalues of the Bethe-Salpeter equation for multiple Bi2212 samples. The leading d-wave eigenvalue increases as the temperature is decreased toward $T_c$, reaching a value of approximately 1 at the $T_c$ corresponding to each doping value. This suggests that spin fluctuations can approximately account for $T_c$ and mediate pairing in the cuprate superconductors.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Stabilizing Fluctuating Spin-Triplet Superconductivity in Graphene via Induced Spin-Orbit Coupling
A recent experiment showed that a proximity-induced Ising spin-orbit coupling enhances the spin-triplet superconductivity in Bernal bilayer graphene. Here, in this work, we show that, due to the nearly perfect spin rotation symmetry of graphene, the fluctuations of the spin orientation of the triplet order parameter suppress the superconducting transition to nearly zero temperature. Our analysis shows that both an Ising spin-orbit coupling and an in-plane magnetic field can eliminate these low-lying fluctuations and can greatly enhance the transition temperature, consistent with the recent experiment. Our model also suggests the possible existence of a phase at small anisotropy and magnetic field which exhibits quasilong-range ordered spin-singlet charge 4e superconductivity, even while the triplet 2e superconducting order only exhibits short-ranged correlations. Finally, we discuss relevant experimental signatures.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Frontiers in Magnetic Materials
Magnetism is crucial to many modern technologies, a driver for condensed matter physics research and one of the most remarkable and diverse properties of matter. We propose to develop understanding of novel magnetism and magnetic related behavior in materials and use this to accelerate the discovery of forefront magnetic materials. The approach is via the connection of magnetic properties to specific structures and materials. Topics that will be addressed are (1) Metallic magnetic materials with unusually low carrier concentrations and/or moments (2) Magnetism arising from unusual chemistry including 4d and 5d magnetism and (3) Materials with strong spin-fluctuations, which can lead to quantum criticality, spin-fluctuation induced superconductivity and other novel quantum behavior. These topics overlap, for example, the 4d ruthenates include ferromagnets (perovskite SrRuO 3 ), extremely high ordering temperature antiferromagnets (honeycomb lattice SrRu 2 O 6 ) and well as quantum materials with strong spin fluctuations (layered perovskite Sr 2 RuO 4 and Sr 3 Ru 2 O 7 ). We will use of density calculations to connect magnetic properties with chemistry and structure and employ phenomenological theories to extend these results to properties that are not directly given by direct first principles methods and we will conduct tests to explore the limitations of density functional approximations and new functionals.
36 MATERIALS SCIENCE↗
Disentangling the role of bond lengths and orbital symmetries in controlling $T_c$ of optimally doped YBa 2 Cu 3 O 7
Optimally doped YBa 2 Cu 3 O 7 (YBCO) has a high critical temperature, at 92 K. It is largely believed that Cooper pairs form in YBCO and other cuprates because of spin fluctuations, but the issue and the detailed mechanism are far from settled. In the present work, we employ a state-of-the-art first-principles ability to compute both the low- and high-energy spin fluctuations in optimally doped YBCO. We benchmark our results against recent inelastic neutron scattering and resonant inelastic x-ray scattering measurements. Further, we use strain as an external parameter to modulate the spin fluctuations and superconductivity. We disentangle the roles of barium-apical oxygen hybridization, interlayer coupling, and orbital symmetries by applying an idealized strain, and also a strain with a fully relaxed structure. We show that shortening the distance between Cu layers is conducive to enhanced Fermi surface nesting, which increases spin fluctuations and drives up $T_c$. However, when the structure is fully relaxed, electrons flow to the $d_{z^2}$ orbital as a consequence of a shortened Ba-O bond, which is detrimental for superconductivity.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
Slow spin dynamics in the hyperhoneycomb lattice [ ( C 2 H 5 ) 3 NH ] 2 Cu 2 ( C 2 O 4 ) 3 revealed by H 1 NMR studies
We report the results of magnetic susceptibility χ and H 1 nuclear magnetic resonance (NMR) measurements on a three-dimensional hyperhoneycomb lattice compound [ ( C 2 H 5 ) 3 NH ] 2 Cu 2 ( C 2 O 4 ) 3 (CCCO). The average value of the antiferromagnetic (AFM) exchange coupling between the Cu 2 + ( S = 1 / 2 ) spins was determined to be J ~ 50 K from the χ measurements. No long-range magnetic ordering has been observed down to T = 50 mK, although NMR lines become slightly broader at low temperatures below 1 K. The broadening of the NMR spectrum observed below 1 K reveals that the Cu spin moments remain at this temperature, suggesting a non-spin-singlet ground state. The temperature and magnetic field dependence of 1 / T 1 at temperatures above 20 K is well explained by paramagnetic thermal spin fluctuations where the fluctuation frequency of Cu 2 + spins is higher than the NMR frequency of the order of megahertz. However, a clear signature of the slowing down of the Cu 2 + spin fluctuations was observed at low temperatures where 1 / T 1 shows a thermally activated behavior. The magnetic field dependence of the magnitude of the spin excitation gap suggests that the magnetic behaviors of CCCO are characterized as an AFM chain at low temperatures.
1-dimensional systems↗
Bogoliubov quasiparticle on the gossamer Fermi surface in electron-doped cuprates
Electron-doped cuprates consistently exhibit strong antiferromagnetic correlations, leading to the prevalent belief that antiferromagnetic spin fluctuations mediate Cooper pairing in these unconventional superconductors. However, early investigations showed that although antiferromagnetic spin fluctuations create the largest pseudogap at hot spots in momentum space, the superconducting gap is also maximized at these locations. This presented a paradox for spin-fluctuation-mediated pairing: Cooper pairing is strongest at momenta where the normal-state low-energy spectral weight is most suppressed. Here we investigate this paradox and find evidence that a gossamer—meaning very faint—Fermi surface can provide an explanation for these observations. We study Nd 2–x Ce x CuO 4 using angle-resolved photoemission spectroscopy and directly observe the Bogoliubov quasiparticles. First, we resolve the previously observed reconstructed main band and the states gapped by the antiferromagnetic pseudogap around the hot spots. Within the antiferromagnetic pseudogap, we also observe gossamer states with distinct dispersion, from which coherence peaks of Bogoliubov quasiparticles emerge below the superconducting critical temperature. Moreover, the direct observation of a Bogoliubov quasiparticle permits an accurate determination of the superconducting gap, yielding a maximum value an order of magnitude smaller than the pseudogap, establishing the distinct nature of these two gaps. Here we propose that orientation fluctuations in the antiferromagnetic order parameter are responsible for the gossamer states.
36 MATERIALS SCIENCE↗
Hole-like Fermi surface in the overdoped non-superconducting Bi 1.8 Pb 0.4 Sr 2 CuO 6+δ
In high-temperature cuprate superconductors, the anti-ferromagnetic spin fluctuations are thought to have a very important role in naturally producing an attractive interaction between the electrons in the d-wave channel. The connection between superconductivity and spin fluctuations is expected to be especially consequential at the overdoped end point of the superconducting dome. In some materials, that point seems to coincide with a Lifshitz transition, where the Fermi surface changes from the hole-like centered at $(\pi, \pi)$ to the electron-like, centered at the Γ point causing a loss of large momentum anti-ferromagnetic fluctuations. In this work, we study the doping dependence of the electronic structure of Bi 1.8 Pb 0.4 Sr 2 CuO$_{6+\delta}$ in angle-resolved photoemission and find that the superconductivity vanishes at lower doping than that at which the Lifshitz transition occurs. This requires a more detailed re-examination of a spin fluctuation scenario.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Solid-state platform for cooperative quantum dynamics driven by correlated emission
While traditionally regarded as an obstacle to quantum coherence, recent breakthroughs in quantum optics have shown that the dissipative interaction of a qubit with its environment can be leveraged to protect quantum states and synthesize many-body entanglement. Inspired by this progress, here we set the stage for the—as yet uncharted—exploration of analogous cooperative phenomena in hybrid solid-state platforms. We develop a comprehensive formalism for the quantum many-body dynamics of an ensemble of solid-state spin defects interacting with the magnetic field fluctuations of a common solid-state reservoir. Our framework applies to any solid-state reservoir whose fluctuating spin, pseudospin, or charge degrees of freedom generate magnetic fields. To understand whether correlations induced by dissipative processes can play a relevant role in a realistic experimental setup, we apply our model to a qubit array interacting via the spin fluctuations of a ferromagnetic bath. Our results show that the low-temperature collective relaxation rates of the qubit ensemble can display clear signatures of super- and subradiance, i.e., forms of cooperative dynamics traditionally achieved in atomic ensembles. We find that the solid-state analog of these cooperative phenomena is robust against spatial disorder in the qubit ensemble and thermal fluctuations of the magnetic reservoir, providing a route for their feasibility in near-term experiments. Finally, our work lays the foundation for a multiqubit approach to quantum sensing of solid-state systems and the direct generation of many-body entanglement in spin-defect ensembles. Furthermore, we discuss how the tunability of solid-state reservoirs opens up novel pathways for exploring cooperative phenomena in regimes beyond the reach of conventional quantum optics setups.
NV centers↗
Large anomalous Hall conductivity induced by spin chirality fluctuation in an ultraclean frustrated antiferromagnet PdCrO 2
Magnetic frustration, realized in the special geometrical arrangement of localized spins, often promotes topologically nontrivial spin textures in the real space and induces significantly large unconventional Hall responses. This spin Berry curvature effect in itinerant frustrated magnets mainly works with a static spin order, limiting the effective temperature range below the magnetic transition temperature and yielding the typical anomalous Hall conductivity below ~ 10 3 Ω -1 cm -1 . Here we show that an ultraclean triangular-lattice antiferromagnet PdCrO 2 exhibits a large anomalous Hall conductivity up to ~ 10 6 Ω -1 cm -1 in the paramagnetic state, which is maintained far above the Neel temperature (T N ) up to ~ 4T N . The reported enhancement of anomalous Hall response above T N is attributed to the skew scattering of highly mobile Pd electrons to fluctuating but locally-correlated Cr spins with a finite spin chirality. Our findings point at an alternative route to realizing high-temperature giant anomalous Hall responses, exploiting magnetic frustration in the ultraclean regime.
36 MATERIALS SCIENCE↗
Static magnetic order with strong quantum fluctuations in spin-1/2 honeycomb magnet Na 2 Co 2 TeO 6
Kitaev interactions, arising from the interplay of frustration and bond anisotropy, can lead to strong quantum fluctuations and, in an ideal case, to a quantum-spin-liquid state. However, in many nonideal materials, spurious non-Kitaev interactions typically promote a zigzag antiferromagnetic order in the d-orbital transition-metal compounds. Here, by combining neutron scattering with muon-spin rotation and relaxation techniques, we provide mechanism insights into the exotic properties of Na 2 Co 2 TeO 6 , a candidate material of the Kitaev model. Below T N , the zero-field muon-spin relaxation rate becomes almost constant (~0.45 μs –1 ). We attribute this temperature-independent relaxation rate to the strong quantum fluctuations, as well as to the frustrated Kitaev interactions. As the magnetic field increases, neutron scattering data indicate a broader spin-wave excitation at the K-point. Therefore, quantum fluctuations seem not only robust but are even enhanced by the applied magnetic field. Our findings provide valuable hints for understanding the onset of the quantum-spin-liquid state in Kitaev materials.
36 MATERIALS SCIENCE↗
Interlayer pairing in bilayer nickelates
The discovery of T c ~ 80 K superconductivity in pressurized La 3 Ni 2 O 7 has launched a new platform to study high-temperature superconductivity. Using non-perturbative dynamic cluster approximation quantum Monte Carlo calculations, we characterize the magnetic and superconducting pairing behavior of a realistic bilayer two-orbital Hubbard-Hund model of this system that describes the relevant Ni e g states with physically relevant interaction strengths. We find a leading s ± superconducting instability in this model at a temperature T ~ 100 K close to the experimentally observed T c . Analyzing the orbital and spatial structure of the effective pairing interaction giving rise to this state reveals that the interaction predominantly acts between local interlayer pairs of the $d_{3z^2-r^2}$ orbital. By correlating the strength of the interaction with that of the magnetic spin fluctuations we show that it is driven by strong interlayer spin-fluctuations arising from the $d_{3z^2-r^2}$ orbital. These results provide first-time non-perturbative evidence supporting the picture that a simple single-orbital bilayer Hubbard model for the Ni $d_{3z^2-r^2}$ orbital provides an excellent low-energy effective description of the superconducting behavior of La 3 Ni 2 O 7 .
Maier, Thomas A. [Oak Ridge National Laboratory (O↗
Scanning SQUID study of ferromagnetism and superconductivity in infinite-layer nickelates
Infinite-layer nickelates R 1-x Sr x NiO 2 (R = La, Pr, Nd) are a class of superconductors with structural similarities to cuprates. Although long-range antiferromagnetic order has not been observed for these materials, magnetic effects such as antiferromagnetic spin fluctuations and spin-glass behavior have been reported. Different experiments have drawn different conclusions about whether the pairing symmetry is s or d wave. In this paper, we applied a scanning superconducting quantum interference device (SQUID) to probe the magnetic behavior of film samples of three infinite-layer nickelates (La 0.85 Sr 0.15 NiO 2 , Pr 0.8 Sr 0.2 NiO 2 , and Nd 0.775 Sr 0.225 NiO 2 ) grown on SrTiO 3 (STO), each with a nominal thickness of 20 unit cells. In all three films, we observed a ferromagnetic background. We also measured the magnetic susceptibility above the superconducting critical temperature in Pr 0.8 Sr 0.2 NiO 2 and La 0.85 Sr 0.15 NiO 2 and identified a non-Curie-Weiss dynamic susceptibility. Both magnetic features are likely due to NiO x nanoparticles. We investigated superconductivity in Pr 0.8 Sr 0.2 NiO 2 and Nd 0.775 Sr 0.225 NiO 2 , which exhibited inhomogeneous diamagnetic screening. The superfluid density inferred from the diamagnetic susceptibility in relatively homogeneous regions shows T-linear behavior in both samples. Finally, we observed superconducting vortices in Nd 0.775 Sr 0.225 NiO 2 . We determined a Pearl length of 330 µm for Nd 0.775 Sr 0.225 NiO 2 at 300 mK, both from the strength of the diamagnetism and from the size and shape of the vortices. These results highlight the importance of considering NiO x particles when interpreting experimental results for these films.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Bayesian experimental design and parameter estimation for ultrafast spin dynamics
Abstract Advanced experimental measurements are crucial for driving theoretical developments and unveiling novel phenomena in condensed matter and materials physics, which often suffer from the scarcity of large-scale facility resources, such as x-ray or neutron scattering centers. To address these limitations, we introduce a methodology that leverages the Bayesian optimal experimental design paradigm to efficiently uncover key quantum spin fluctuation parameters from x-ray photon fluctuation spectroscopy (XPFS) data. Our method is compatible with existing theoretical simulation pipelines and can also be used in combination with fast machine learning surrogate models in the event that real-time simulations are unfeasible. Our numerical benchmarks demonstrate the superior performance in predicting model parameters and in delivering more informative measurements within limited experimental time. Our method can be adapted to many different types of experiments beyond XPFS and spin fluctuation studies, facilitating more efficient data collection and accelerating scientific discoveries.
97 MATHEMATICS AND COMPUTING↗
Neutron scattering study of fluctuating and static spin correlations in the anisotropic spin glass Fe 2 Ti O 5
The anisotropic spin-glass transition, in which spin freezing is observed only along the c axis in pseudobrookite Fe 2 TiO 5 , has long been perplexing because the Fe 3+ moments (d 5 ) are expected to be isotropic. Recently, neutron diffraction demonstrated that surfboard-shaped antiferromagnetic nanoregions coalesce above the glass transition temperature T g ≈55K, and a model was proposed in which the freezing of the surfboard magnetization fluctuations leads to the anisotropic spin-glass state. Given this model, we have carried out high-resolution inelastic neutron scattering measurements of the spin-spin correlations to understand the temperature dependence of the intrasurfboard spin dynamics on neutron (picosecond) timescales. Here, in this paper, we report on the temperature-dependence of the spin fluctuations measured from single-crystal Fe 2 TiO 5 . Strong quasi-elastic magnetic scattering, arising from intrasurfboard correlations, is observed well above T g . The spin fluctuations possess a steep energy–wave vector relation and are indicative of strong exchange interactions, consistent with the large Curie-Weiss temperature. As the temperature approaches T g from above, a shift in spectral weight from inelastic to elastic scattering is observed. At various temperatures between 4 and 300 K, a characteristic relaxation rate of the fluctuations is determined. Despite the freezing of most of the spin correlations, an inelastic contribution remains even at base temperature, signifying the presence of fluctuating intrasurfboard spin correlations to at least T/T g ≈0.1 , consistent with an energy landscape that is a hybrid between conventional and geometrically frustrated spin glasses.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Evolution of spin excitations from bulk to monolayer FeSe
Abstract In ultrathin films of FeSe grown on SrTiO 3 (FeSe/STO), the superconducting transition temperature T c is increased by almost an order of magnitude, raising questions on the pairing mechanism. As in other superconductors, antiferromagnetic spin fluctuations have been proposed to mediate SC making it essential to study the evolution of the spin dynamics of FeSe from the bulk to the ultrathin limit. Here, we investigate the spin excitations in bulk and monolayer FeSe/STO using resonant inelastic x-ray scattering (RIXS) and quantum Monte Carlo (QMC) calculations. Despite the absence of long-range magnetic order, bulk FeSe displays dispersive magnetic excitations reminiscent of other Fe-pnictides. Conversely, the spin excitations in FeSe/STO are gapped, dispersionless, and significantly hardened relative to its bulk counterpart. By comparing our RIXS results with simulations of a bilayer Hubbard model, we connect the evolution of the spin excitations to the Fermiology of the two systems revealing a remarkable reconfiguration of spin excitations in FeSe/STO, essential to understand the role of spin fluctuations in the pairing mechanism.
36 MATERIALS SCIENCE↗
Electronic structure, and magnetic and superconducting pairing tendencies of the alternating single layer–bilayer stacking nickelate La 5 Ni 3 O 11 under pressure
Nickelates have continued to surprise since their unconventional superconductivity was discovered. Recently, the layered nickelate La 5 Ni 3 O 11 with hybrid single-layer and bilayer stacking showed superconductivity under high pressure. This compound combines features of single-layer La 2 NiO 4 and bilayer La 3 Ni 2 O 7 , but its pairing mechanism remains to be understood. Motivated by this finding, here we report a comprehensive theoretical study of this system. Our density functional theory calculations reveal that the undistorted P4/mmm phase without pressure is unstable due to three distortion modes. As pressure increases, these modes are suppressed, leading to the high-symmetry P4/mmm phase without NiO 6 octahedron tilting. Moreover, the “charge transfer” between the single-layer and bilayer sublattices was observed, leading to hole doping in the single-layer blocks. Our random-phase approximation calculations indicate a leading 𝑑 𝑥 2 −𝑦 2 -wave pairing state that arises from spin-fluctuation scattering between Fermi surface states mainly originating from the single-layer blocks and additional weaker contributions from the bilayer blocks. These spin fluctuations could be detected by inelastic neutron scattering as a strong peak at 𝐪 = (𝜋,𝜋). Our findings distinguish La 5 Ni 3 O 11 from other nickelate superconductors discovered so far and the high-𝑇 𝑐 cuprates. We also discuss both similarities and differences between La 5 Ni 3 O 11 and other hybrid stacking nickelates.
Zhang, Yang [Univ. of Tennessee, Knoxville, TN (Un↗
Gapped commensurate antiferromagnetic response in a strongly underdoped model cuprate superconductor
It is a distinct possibility that spin fluctuations are the pairing interactions in numerous unconventional superconductors. In the high-transition-temperature (high-T c ) cuprates, superconductivity emerges upon doping antiferromagnetic Mott insulators, and spin fluctuations might furthermore drive unusual pseudogap phenomena. Here we use magnetic neutron scattering to study the highly underdoped cuprate HgBa 2 CuO 4+δ (hole concentration p ≈ 0.064). In contrast to prior results for other underdoped cuprates, we find no evidence of incommensurate magnetic order associated with spin-density-wave or stripe correlations. Instead, the antiferromagnetic response in both the superconducting and pseudogap states is gapped below Δ AF ≈ 6 meV, commensurate over a wide energy range, and disperses above about 55 meV. Given the pristine nature of HgBa 2 CuO 4+δ , which exhibits high structural symmetry and minimal point disorder effects, this behavior likely signifies the unmasked response of the underlying CuO 2 planes near the Mott-insulating state. These results serve as a benchmark for a refined theoretical understanding of the cuprates.
Materials science↗