arXiv subjects

B. Keimer

Publications and source records attributed to B. Keimer.

At least 73 records · Page 4Linked to original sources

arXiv2020

Charge density waves in YBa$_2$Cu$_3$O$_{6.67}$ probed by resonant x-ray scattering under uniaxial compression

We report a comprehensive Cu L$_3$-edge resonant x-ray scattering study of two- and three-dimensional (2D and 3D) incommensurate charge correlations in single crystals of the underdoped high-temperature superconductor YBa$_2$Cu$_3$O$_{6.67}$ under uniaxial compression up to 1% along the two inequivalent Cu-O-Cu bond directions (a and b) in the CuO$_2$ planes. The pressure response of the 2D charge correlations is symmetric: pressure along a enhances correlations along b, and vice versa. Our results imply that the underlying order parameter is uniaxial. In contrast, 3D long-range charge order is only observed along b in response to compression along a. Spectroscopic resonant x-ray scattering measurements show that the 3D charge order resides exclusively in the CuO$_2$ planes and may thus be generic to the cuprates. We discuss implications of these results for models of electronic nematicity and for the interplay between charge order and superconductivity.

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arXiv2020

Approaching two-dimensional superconductivity in ultrathin DyBa$_2$Cu$_3$O$_{7-δ}$

The temperature dependence of the superfluid density $ρ_s(T)$ has been measured for a series of ultrathin MBE-grown DyBa$_2$Cu$_3$O$_{7-δ}$ superconducting (SC) films by sub-mm wave interferometry combined with time-domain THz spectroscopy and IR ellipsometry. We find that all films 10 u.c. and thicker show the same universal temperature dependence of $ρ_s(T)$, which follows the critical behavior characteristic of single crystal YBa$_2$Cu$_3$O$_{7-δ}$ as $T$ approaches $T_c$. In 7 u.c. thick films, $ρ_s(T)$ declines steeply upon approaching $T_c$, as expected for the Berezinskii-Kosterlitz-Thouless vortex unbinding transition. Our analysis provides evidence for a sharply defined 4 u.c. non-SC interfacial layer, leaving a quasi-2D SC layer on top. We propose that the SC state in this interfacial layer is suppressed by competing (possibly charge) order.

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arXiv2020

Parametrically amplified phase-incoherent superconductivity in YBa$_2$Cu$_3$O$_{6+x}$

The possibility of enhancing desirable functional properties of complex materials by optical driving is motivating a series of studies of their nonlinear terahertz response. In high-Tc cuprates, large amplitude excitation of certain infrared-active lattice vibrations has been shown to induce transient features in the reflectivity suggestive of non-equilibrium superconductivity. Yet, a microscopic mechanism for these observations is still lacking. Here, we report measurements of time- and scattering-angle-dependent second-harmonic generation in YBa$_2$Cu$_3$O$_{6+x}$, taken under the same excitation conditions that result in superconductor-like terahertz reflectivity. We discover a three-order-of-magnitude amplification of a 2.5-terahertz electronic mode, which is unique because of its symmetry, momentum, and temperature dependence. A theory for parametric three-wave amplification of Josephson plasmons, which are assumed to be well-formed below T$_c$ but overdamped throughout the pseudogap phase, explains all these observations and provides a mechanism for non-equilibrium superconductivity. More broadly, our work underscores the role of parametric mode mixing to stabilize fluctuating orders in quantum materials.

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arXiv2020

Inhomogeneous ferromagnetism mimics signatures of the topological Hall effect in SrRuO$_3$ films

Topological transport phenomena in magnetic materials are a major topic of current condensed matter research. One of the most widely studied phenomena is the ``topological Hall effect'' (THE), which is generated via spin-orbit interactions between conduction electrons and topological spin textures such as skyrmions. We report a comprehensive set of Hall effect and magnetization measurements on epitaxial films of the prototypical ferromagnetic metal SrRuO$_3$ the magnetic and transport properties of which were systematically modulated by varying the concentration of Ru vacancies. We observe Hall effect anomalies that closely resemble signatures of the THE, but a quantitative analysis demonstrates that they result from inhomogeneities in the ferromagnetic magnetization caused by a non-random distribution of Ru vacancies. As such inhomogeneities are difficult to avoid and are rarely characterized independently, our results call into question the identification of topological spin textures in numerous prior transport studies of quantum materials, heterostructures, and devices. Firm conclusions regarding the presence of such textures must meet stringent conditions such as probes that couple directly to the non-collinear magnetization on the atomic scale.

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arXiv2020

Pump frequency resonances for light-induced incipient superconductivity in YBa$_2$Cu$_3$O$_{6.5}$

Optical excitation in the cuprates has been shown to induce transient superconducting correlations above the thermodynamic transition temperature, $T_C$, as evidenced by the terahertz frequency optical properties in the non-equilibrium state. In YBa$_2$Cu$_3$O$_{6+x}$ this phenomenon has so far been associated with the nonlinear excitation of certain lattice modes and the creation of new crystal structures. In other compounds, like La$_{2-x}$Ba$_x$CuO$_4$, similar effects were reported also for excitation at near infrared frequencies, and were interpreted as a signature of the melting of competing orders. However, to date it has not been possible to systematically tune the pump frequency widely in any one compound, to comprehensively compare the frequency dependent photo-susceptibility for this phenomenon. Here, we make use of a newly developed optical parametric amplifier, which generates widely tunable high intensity femtosecond pulses, to excite YBa$_2$Cu$_3$O$_{6.5}$ throughout the entire optical spectrum (3 - 750 THz). In the far-infrared region (3 - 25 THz), signatures of non-equilibrium superconductivity are induced only for excitation of the 16.4 THz and 19.2 THz vibrational modes that drive $c$-axis apical oxygen atomic positions. For higher driving frequencies (25 - 750 THz), a second resonance is observed around the charge transfer band edge at ~350 THz. These observations highlight the importance of coupling to the electronic structure of the CuO$_2$ planes, either mediated by a phonon or by charge transfer.

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arXiv2020

Spin-wave gap collapse in Rh-doped Sr2IrO4

We use resonant inelastic x-ray scattering (RIXS) at the Ir L3 edge to study the effect of hole doping upon the Jeff=1/2 Mott-insulating state in Sr2IrO4, via Rh replacement of the Ir site. The spin-wave gap, associated with XY-type spin-exchange anisotropy, collapses with increasing Rh content, prior to the suppression of the Mott-insulating state and in contrast to electron doping via La substitution of the Sr site. At the same time, despite heavy damping, the d-d excitation spectra retain their overall amplitude and dispersion character. A careful study of the spin-wave spectrum reveals that deviations from the J1-J2-J3 Heisenberg used to model the pristine system disappear at intermediate doping levels. These findings are interpreted in terms of a modulation of Ir-Ir correlations due to the influence of Rh impurities upon nearby Ir wave functions, even as the single-band Jeff=1/2 model remains valid up to full carrier delocalization. They underline the importance of the transition metal site symmetry when doping pseudospin systems such as Sr2IrO4.

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arXiv2019

Proximity effect in [Nb(1.5nm)/Fe(x)]$_{10}$/Nb(50nm) superconducting/ferromagnet heterostructures

We have investigated the structural, magnetic and superconducting properties of [Nb(1.5nm)/Fe(x)]$_{10}$ superlattices deposited on a thick Nb(50nm) layer. Our investigation showed that the Nb(50nm) layer grows epitaxially at 800$^\circ$C on Al$_2$O$_3$(1$\bar{1}$02) substrate. Samples grown at this condition posses a high residual resistivity ratio of 15-20. By using neutron reflectometry we show that Fe/Nb superlattices with $x<$ 4 nm form a depth-modulated FeNb alloy with concentration of iron varying between 60% and 90%. This alloy has properties of a weak ferromagnet. Proximity of this weak ferromagnetic layer to a thick superconductor leads to an intermediate phase that is characterized by co-existing superconducting and normal-state domains. By increasing the thickness of the Fe layer to $x$ = 4 nm the intermediate phase disappears. We attribute the intermediate state to proximity induced non-homogeneous superconductivity in the periodic Fe/Nb structure.

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arXiv2019

Backfolded acoustic phonons in metal-oxide superlattices

We report the observation of low-frequency modes in the Raman spectra of thin-film superlattices of the high-temperature superconductor YBa$ _{2} $Cu$ _{3} $O$ _{7-δ} $ and various manganite perovskites. Our study shows that these modes are caused by the backfolding of acoustic phonons due to the additional periodicity introduced by the superlattice. Such modes were previously only observed for ultra-pure semiconductor superlattices. They can be used to determine the bilayer thickness of the superlattice and its speed of sound. Moreover, we use the spatial resolution of Raman microscopy to map the film thickness inhomogeneity across a sample, making these modes a useful tool to characterize thin-film superlattices.

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arXiv2019

Electronic and vibrational signatures of ruthenium vacancies in Sr$_2$RuO$_4$ thin films

The synthesis of stoichiometric Sr$_2$RuO$_4$ thin films has been a challenge because of the high volatility of ruthenium oxide precursors, which gives rise to ruthenium vacancies in the films. Ru vacancies greatly affect the transport properties and electronic phase behavior of Sr$_2$RuO$_4$, but their direct detection is difficult due to their atomic dimensions and low concentration. We applied polarized X-ray absorption spectroscopy at the oxygen K-edge and confocal Raman spectroscopy to Sr$_2$RuO$_4$ thin films synthesized under different conditions. The results show that these methods can serve as sensitive probes of the electronic and vibrational properties of Ru vacancies, respectively. The intensities of the vacancy-related spectroscopic features extracted from these measurements are well correlated with the transport properties of the films. The methodology introduced here can thus help to understand and control the stoichiometry and transport properties in films of Sr$_2$RuO$_4$ and other ruthenates.

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arXiv2019

Compressive-strain induced enhancement of exchange interactions and short-range magnetic order in Sr$_2$IrO$_4$ investigated by Raman spectroscopy

We have carried out Raman spectroscopy experiments to investigate two-magnon excitations in epitaxial thin films of the quasi-two-dimensional antiferromagnetic Mott insulator Sr$_2$IrO$_4$ under in-plane misfit strain. With in-plane biaxial compression, the energy of the two-magnon peak increases, and the peak remains observable over a wider temperature range above the Néel temperature, indicating strain-induced enhancement of the superexchange interactions between $\it{J}_{eff}$ = 1/2 pseudospins. From density functional theory calculations, we have found an increase of the nearest-neighbor hopping parameter and exchange interaction with increasing biaxial compressive strain, in agreement with the experimental observations. Our experimental and theoretical results provide perspectives for systematic, theory-guided strain control of the primary exchange interactions in 5$\it{d}$ transition metal oxides.

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arXiv2019

Raman scattering from current-stabilized nonequilibrium phases in Ca$_2$RuO$_4$

We used Raman light scattering to study the current-stabilized nonequilibrium semimetallic and metallic phases in Ca$_2$RuO$_4$. By determining the local temperature through careful analysis of the Stokes and anti-Stokes intensities, we find that Joule heating can be completely avoided by supplying sufficient cooling power in a helium-flow cryostat, and that the current induces the semimetallic state without inducing any significant heating. We further investigate the current-induced semimetallic state as a function of temperature and current. We confirm the absence of long-range antiferromagnetic order and identify a substantial Fano broadening of several phonons, which suggests coupling to charge and orbital fluctuations. Our results demonstrate that the semimetallic state is a genuine effect of the applied electrical current and that the current-induced phases have characteristics distinct from the equilibrium ones.

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arXiv2019

Observation of spin-orbit excitations and Hund's multiplets in Ca$_2$RuO$_4$

We use Ru $L_3$-edge (2838.5 eV) resonant inelastic x-ray scattering (RIXS) to quantify the electronic structure of Ca$_2$RuO$_4$, a layered $4d$-electron compound that exhibits a correlation-driven metal-insulator transition and unconventional antiferromagnetism. We observe a series of Ru intra-ionic transitions whose energies and intensities are well described by model calculations. In particular, we find a $\rm{J}=0\rightarrow 2$ spin-orbit excitation at 320 meV, as well as Hund's-rule driven $\rm{S}=1\rightarrow 0$ spin-state transitions at 750 and 1000 meV. The energy of these three features uniquely determines the spin-orbit coupling, tetragonal crystal-field energy, and Hund's rule interaction. The parameters inferred from the RIXS spectra are in excellent agreement with the picture of excitonic magnetism that has been devised to explain the collective modes of the antiferromagnetic state. $L_3$-edge RIXS of Ru compounds and other $4d$-electron materials thus enables direct measurements of interactions parameters that are essential for realistic model calculations.

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arXiv2019

A Unique Crystal Structure of Ca$_2$RuO$_4$ in the Current Stabilized Semi-Metallic State

The electric-current stabilized semi-metallic state in the quasi-two-dimensional Mott insulator Ca$_2$RuO$_4$ exhibits an exceptionally strong diamagnetism. Through a comprehensive study using neutron and X-ray diffraction, we show that this non-equilibrium phase assumes a crystal structure distinct from those of equilibrium metallic phases realized in the ruthenates by chemical doping, high pressure and epitaxial strain, which in turn leads to a distinct electronic band structure. Dynamical mean field theory calculations based on the crystallographically refined atomic coordinates and realistic Coulomb repulsion parameters indicate a semi-metallic state with partially gapped Fermi surface. Our neutron diffraction data show that the non-equilibrium behavior is homogeneous, with antiferromagnetic long-range order completely suppressed. These results provide a new basis for theoretical work on the origin of the unusual non-equilibrium diamagnetism in Ca$_2$RuO$_4$.

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arXiv2019

Resonant inelastic x-ray scattering study of bond order and spin excitations in nickelate thin-film structures

We used high-resolution resonant inelastic x-ray scattering (RIXS) at the Ni $L_3$ edge to simultaneously investigate high-energy interband transitions characteristic of Ni-O bond ordering and low-energy collective excitations of the Ni spins in the rare-earth nickelates $R$NiO$_3$ ($R$ = Nd, Pr, La) with pseudocubic perovskite structure. With the support of calculations based on a double-cluster model we quantify bond order (BO) amplitudes for different thin films and heterostructures and discriminate short-range BO fluctuations from long-range static order. Moreover we investigate magnetic order and exchange interactions in spatially confined $R$NiO$_3$ slabs by probing dispersive magnon excitations. While our study of superlattices (SLs) grown in the (001) direction of the perovskite structure reveals a robust non-collinear spin spiral magnetic order with dispersive magnon excitations that are essentially unperturbed by BO modulations and spatial confinement, we find magnons with flat dispersions and strongly reduced energies in SLs grown in the $(111)_{\text{pc}}$ direction that exhibit collinear magnetic order. These results give insight into the interplay of different collective ordering phenomena in a prototypical 3$d$ transition metal oxide and establish RIXS as a powerful tool to quantitatively study several order parameters and the corresponding collective excitations within one experiment.

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arXiv2019

Spin waves and spin-state transitions in a ruthenate high-temperature antiferromagnet

Ruthenium compounds play prominent roles in materials research ranging from oxide electronics to catalysis, and serve as a platform for fundamental concepts such as spin-triplet superconductivity, Kitaev spin-liquids, and solid-state analogues of the Higgs mode in particle physics. However, basic questions about the electronic structure of ruthenates remain unanswered, because several key parameters (including the Hund's-rule, spin-orbit, and exchange interactions) are comparable in magnitude, and their interplay is poorly understood - partly due to difficulties in synthesizing sizable single crystals for spectroscopic experiments. Here we introduce a resonant inelastic x-ray scattering (RIXS) technique capable of probing collective modes in microcrystals of $4d$-electron materials. We present a comprehensive set of data on spin waves and spin-state transitions in the honeycomb antiferromagnet SrRu$_{2}$O$_{6}$, which possesses an unusually high Néel temperature. The new RIXS method provides fresh insight into the unconventional magnetism of SrRu$_{2}$O$_{6}$, and enables momentum-resolved spectroscopy of a large class of $4d$ transition-metal compounds.

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arXiv2019

Magnetic proximity effect in [Nb/Gd] superlattices seen by neutron scattering

We have used spin-polarized neutron reflectometry to investigate the magnetization profile of superlattices composed of ferromagnetic Gd and superconducting Nb layers. We have observed a partial suppression of ferromagnetic (F) order of Gd layers in [Gd($d_F$)/Nb(25nm)]$_{12}$ superlattices below the superconducting (S) transition of the Nb layers. The amplitude of the suppression decreases with increasing $d_F$. By analyzing the neutron spin asymmetry we conclude that the observed effect has an electromagnetic origin - the proximity-coupled S layers screen out the external magnetic field and thus suppress the F response of the Gd layers inside the structure. Our investigation demonstrates the considerable influence of electromagnetic effects on the magnetic properties of S/F systems.

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arXiv2019

Polarization resolved Cu $L_3$-edge resonant inelastic x-ray scattering of orbital and spin excitations in NdBa$_{2}$Cu$_{3}$O$_{7-δ}$

High resolution resonant inelastic x-ray scattering (RIXS) has proven particularly effective in the determination of crystal field and spin excitations in cuprates. Its strength lies in the large Cu $L_{3}$ resonance and in the fact that the scattering cross section follows quite closely the single-ion model predictions, both in the insulating parent compounds and in the superconducting doped materials. However, the spectra become increasingly broader with (hole) doping, hence resolving and assigning spectral features has proven challenging even with the highest energy resolution experimentally achievable. Here we have overcome this limitation by measuring the complete polarization dependence of the RIXS spectra as function of momentum transfer and doping in thin films of NdBa$_{2}$Cu$_{3}$O$_{7-δ}$. Besides confirming the previous assignment of $dd$ and spin excitations (magnon, bimagnon) in the antiferromagnetic insulating parent compound, we unequivocally single out the actual spin-flip contribution at all dopings. We also demonstrate that the softening of $dd$ excitations is mainly attributed to the shift of the $xy$ peak to lower energy loss. These results provide a definitive assessment of the RIXS spectra of cuprates and demonstrate that RIXS measurements with full polarization control are practically feasible and highly informative.

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arXiv2019

Optical Characteristics of Charge Carrier Transfer across Interfaces between YBa$_2$Cu$_3$O$_{6+δ}$ and La$_{0.7}$Ca$_{0.3}$MnO$_3$

We report a spectral ellipsometry study of multilayers composed of superconducting YBa$_2$Cu$_3$O$_{6+δ}$ (YBCO) and ferromagnetic La$_{0.7}$Ca$_{0.3}$MnO$_3$ in the spectral range of 0.7 - 6.5 eV. With increasing YBCO sublayer thickness, the optical spectral weight is enhanced at photon energies of 1.5 - 3.5 eV. The spectral weight enhancement is proportional to the number of interfaces of each multilayer sample, indicating its association with the interfacial electronic structure. Based on calculations in the framework of a multilayer model, we find that the shape of the interface-induced spectral weight is consistent with transfer of hole-carriers from YBCO to LCMO. Our results imply that the holes that are transferred across the interfaces accumulate in the LCMO layers, rather than being pinned by interfacial defects or annihilated by electron donors such as oxygen vacancies. Optical spectroscopy can thus serve as a non-destructive probe of charge transfer across buried interfaces in metal-oxide heterostructures.

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