arXiv subjects

Bernhard Keimer

Publications and source records attributed to Bernhard Keimer.

At least 37 records · Page 2Linked to original sources

arXiv2024

Nature of the current-induced insulator-to-metal transition in Ca$_2$RuO$_4$ as revealed by transport-ARPES

The Mott insulator Ca$_2$RuO$_4$ exhibits a rare insulator-to-metal transition (IMT) induced by DC current. While structural changes associated with this transition have been tracked by neutron diffraction, Raman scattering, and x-ray spectroscopy, work on elucidating the response of the electronic degrees of freedom is still in progress. Here we unveil the current-induced modifications of the electronic states of Ca$_2$RuO$_4$ by employing angle-resolved photoemission spectroscopy (ARPES) in conjunction with four-probe transport. Two main effects emerge: a clear reduction of the Mott gap and a modification in the dispersion of the Ru-bands. The changes in dispersion occur exclusively along the $XM$ high-symmetry direction, parallel to the $b$-axis where the greatest in-plane lattice change occurs. These experimental observations, together with dynamical mean-field theory (DMFT) calculations simulated from the current-induced structural distortions, indicate the intimate interplay of lattice and orbital-dependent electronic response in the current-driven IMT. Furthermore, based on a free energy analysis, we demonstrate that the current-induced phase, albeit thermodynamically equivalent, is electronically distinct from the high-temperature zero-current metallic phase. Our results provide insight into the elusive nature of the current-induced IMT of Ca$_2$RuO$_4$ and advance the challenging, yet powerful, technique of transport-ARPES.

cond-mat.str-el↗

arXiv2024

Electronic structure of the alternating monolayer-trilayer phase of La3Ni2O7

Recent studies of La$_3$Ni$_2$O$_7$ have identified a bilayer (2222) structure and an unexpected alternating monolayer-trilayer (1313) structure, both of which feature signatures of superconductivity near 80 K under high pressures. Using angle-resolved photoemission spectroscopy, we measure the electronic structure of 1313 samples. In contrast to the previously studied 2222 structure, we find that the 1313 structure hosts a flat band with a markedly different binding energy, as well as an additional electron pocket and band splittings. By comparison to local-density approximation calculations, we find renormalizations of the Ni-$d_{z^2}$ and Ni-$d_{x^2-y^2}$ derived bands to be about 5 to 7 and about 4 respectively, suggesting strong correlation effects. These results reveal important differences in the electronic structure brought about by the distinct structural motifs with the same stoichiometry. Such differences may be relevant to the putative high temperature superconductivity.

cond-mat.supr-con↗

arXiv2024

Discovery of Superconductivity and Electron-Phonon Drag in the Non-Centrosymmetric Weyl Semimetal LaRhGe$_3$

We present an exploration of the effect of electron-phonon coupling and broken inversion symmetry on the electronic and thermal properties of the semimetal LaRhGe$_3$. Our transport measurements reveal evidence for electron-hole compensation at low temperatures, resulting in a large magnetoresistance of 3000% at 1.8 K and 14 T. The carrier concentration is on the order of $10^{21}\rm{/cm}^3$ with high carrier mobilities of $2000~\rm{cm}^2/\rm{Vs}$. When coupled to our theoretical demonstration of symmetry-protected $\textit{almost movable}$ Weyl nodal lines, we conclude that LaRhGe$_3$ supports a Weyl semimetallic state. We discover superconductivity in this compound with a $T_{\text c}$ of 0.39(1) K and $B_{\rm{c}}(0)$ of 2.2(1) mT, with evidence from specific heat and transverse-field muon spin relaxation. We find an exponential dependence in the normal state electrical resistivity below $\sim50$ K, while Seebeck coefficient and thermal conductivity measurements each reveal a prominent peak at low temperatures, indicative of strong electron-phonon interactions. To this end, we examine the temperature-dependent Raman spectra of LaRhGe$_3$ and find that the lifetime of the lowest energy $A_1$ phonon is dominated by phonon-electron scattering instead of anharmonic decay. We conclude that LaRhGe$_3$ has strong electron-phonon coupling in the normal state, while the superconductivity emerges from weak electron-phonon coupling. These results open up the investigation of electron-phonon interactions in the normal state of superconducting non-centrosymmetric Weyl semimetals.

cond-mat.supr-con↗

arXiv2024

Magnetic field expulsion in optically driven YBa$_2$Cu$_3$O$_{6.48}$

Coherent optical driving in quantum solids is emerging as a new research frontier, with many demonstrations of exotic non-equilibrium quantum phases. These are based on engineered band structures, and on stimulated nonlinear interactions between driven modes. Enhanced functionalities like ferroelectricity, magnetism and superconductivity have been reported in these non-equilibrium settings. In high-Tc cuprates, coherent driving of certain phonon modes induces a transient state with superconducting-like optical properties, observed far above T$_c$ and throughout the pseudogap phase. Questions remain not only on the microscopic nature of this phenomenon, but also on the macroscopic properties of these transient states, beyond the documented optical conductivities. Crucially, it is not clear if driven cuprates exhibit Meissner-like diamagnetism. Here, the time-dependent magnetic-field amplitude surrounding a driven YBa$_2$Cu$_3$O$_{6.48}$ sample is probed by measuring Faraday rotation in a GaP layer adjacent to the superconductor. For the same driving conditions that result in superconducting-like optical properties, an enhancement of magnetic field at the edge of the sample is detected, indicative of induced diamagnetism. The dynamical field expulsion measured after pumping is comparable in size to the one expected in an equilibrium type II superconductor of similar shape and size with a volume susceptibility $χ_v$ of order -0.3. Crucially, this value is incompatible with a photo-induced increase in mobility without superconductivity. Rather, it underscores the notion of a pseudogap phase in which incipient superconducting correlations are enhanced or synchronized by the optical drive.

cond-mat.supr-con↗

arXiv2024

Using strain to uncover the interplay between two- and three-dimensional charge density waves in high-temperature superconducting YBa$_{2}$Cu$_{3}$O$_{\rm{y}}$

Uniaxial pressure provides an efficient approach to control the competition between charge density waves (CDWs) and superconductivity in underdoped YBa$_{2}$Cu$_{3}$O$_{\rm{y}}$. It can enhance the correlation volume of ubiquitous short-range 2D CDW correlations, and induces a long-range 3D CDW otherwise only accessible at large magnetic fields. Here, we use x-ray diffraction to study the strain and doping evolution of these CDWs. No signatures of discommensurations nor pair density waves are observed in the investigated strain-temperature parameter space, but direct evidence for a form of competition between 2D and 3D CDWs is uncovered. We show that the interplay between the 3D CDW, the 2D CDWs and superconductivity is qualitatively well described by including strain effects in simulations of a nonlinear sigma model of competing superconducting and CDW orders. From a broader perspective, our results underscore the potential of strain tuning as a powerful tool for probing and manipulating competing orders in quantum materials.

cond-mat.supr-con↗

arXiv2024

Spin-orbit excitons in a correlated metal: Raman scattering study of Sr2RhO4

Using Raman spectroscopy to study the correlated 4$d$-electron metal Sr$_2$RhO$_4$, we observe pronounced excitations at 220 meV and 240 meV with $A_\mathrm{1g}$ and $B_\mathrm{1g}$ symmetries, respectively. We identify them as transitions between the spin-orbit multiplets of the Rh ions, in close analogy to the spin-orbit excitons in the Mott insulators Sr$_2$IrO$_4$ and $α$-RuCl$_3$. This observation provides direct evidence for the unquenched spin-orbit coupling in Sr$_2$RhO$_4$. A quantitative analysis of the data reveals that the tetragonal crystal field $Δ$ in Sr$_2$RhO$_4$ has a sign opposite to that in insulating Sr$_2$IrO$_4$, which enhances the planar $xy$ orbital character of the effective $J=1/2$ wave function. This supports a metallic ground state, and suggests that $c$-axis compression of Sr$_2$RhO$_4$ may transform it into a quasi-two-dimensional antiferromagnetic insulator.

cond-mat.str-el↗

arXiv2024

Alternate cleavage structure and electronic inhomogeneity in Ca-doped YBa$_2$Cu$_3$O$_{7-δ}$

YBa$_2$Cu$_3$O$_{7-δ}$ (YBCO) has favorable macroscopic superconducting properties of $T_\mathrm{c}$ up to 93 K and $H_{c2}$ up to 150 T. However, its nanoscale electronic structure remains mysterious because bulk-like electronic properties are not preserved near the surface of cleaved samples for easy access by local or surface-sensitive probes. It has been hypothesized that Ca-doping at the Y site could induce an alternate cleavage plane that mitigates this issue. We use scanning tunneling microscopy (STM) to study both Ca-free and 10% Ca-doped YBCO, and find that the Ca-doped samples do indeed cleave on an alternate plane, yielding a spatially-disordered partial (Y,Ca) layer. Our density functional theory calculations support the increased likelihood of this new cleavage plane in Ca-doped YBCO. On this surface, we image a superconducting gap with average value 24 $\pm$ 3 meV and characteristic length scale 1-2 nm, similar to Bi-based high-$T_\mathrm{c}$ cuprates, but the first map of gap inhomogeneity in the YBCO family.

cond-mat.supr-con↗

arXiv2023

Unconventional crystal structure of the high-pressure superconductor La$_3$Ni$_2$O$_7$

The discovery of high-temperature superconductivity in La$_3$Ni$_2$O$_7$ at pressures above 14 GPa has spurred extensive research efforts. Yet, fundamental aspects of the superconducting phase, including the possibility of a filamentary character, are currently subjects of controversial debates. Conversely, a crystal structure with NiO$_6$ octahedral bilayers stacked along the $c$-axis direction was consistently posited in initial studies on La$_3$Ni$_2$O$_7$. Here we reassess this structure in optical floating zone-grown La$_3$Ni$_2$O$_7$ single crystals that show signs of filamentary superconductivity. Employing scanning transmission electron microscopy and single-crystal x-ray diffraction under high pressures, we observe multiple crystallographic phases in these crystals, with the majority phase exhibiting alternating monolayers and trilayers of NiO$_6$ octahedra, signifying a profound deviation from the previously suggested bilayer structure. Using density functional theory, we disentangle the individual contributions of the monolayer and trilayer structural units to the electronic band structure of La$_3$Ni$_2$O$_7$, providing a firm basis for advanced theoretical modeling and future evaluations of the potential of the monolayer-trilayer structure for hosting superconductivity.

cond-mat.supr-con↗

arXiv2023

Rich Magnetic Phase Diagram of Putative Helimagnet Sr$_3$Fe$_2$O$_7$

The cubic perovskite SrFeO$_3$ was recently reported to host hedgehog- and skyrmion-lattice phases in a highly symmetric crystal structure which does not support the Dzyaloshinskii-Moriya interactions commonly invoked to explain such magnetic order. Hints of a complex magnetic phase diagram have also recently been found in powder samples of the single-layer Ruddlesden-Popper analog Sr$_2$FeO$_4$, so a reinvestigation of the bilayer material Sr$_3$Fe$_2$O$_7$, believed to be a simple helimagnet, is called for. Our magnetization and dilatometry studies reveal a rich magnetic phase diagram with at least 6 distinct magnetically ordered phases and strong similarities to that of SrFeO$_3$. In particular, at least one phase is apparently multiple-$\mathbf{q}$, and the $\mathbf{q}$s are not observed to vary among the phases. Since Sr$_3$Fe$_2$O$_7$ has only two possible orientations for its propagation vector, some of the phases are likely exotic multiple-$\mathbf{q}$ order, and it is possible to fully detwin all phases and more readily access their exotic physics.

cond-mat.str-el↗

arXiv2023

Singlet magnetism in intermetallic UGa$_2$ unveiled by inelastic x-ray scattering

Using high resolution tender-x-ray resonant inelastic scattering and hard-x-ray non-resonant inelastic scattering beyond the dipole limit we were able to detect electronic excitations in intermetallic UGa$_2$ that are highly atomic in nature. Analysis of the spectral lineshape reveals that the local $5f^2$ configuration characterizes the correlated nature of this ferromagnet. The orientation and directional dependence of the spectra indicate that the ground state is made of the $Γ_1$ singlet and/or $Γ_6$ doublet symmetry. With the ordered moment in the $ab$ plane, we infer that the magnetism originates from the higher lying $Γ_6$ doublet being mixed with the $Γ_1$ singlet due to inter-site exchange, qualifying UGa$_2$ to be a true quantum magnet. The ability to observe atomic excitations is crucial to resolve the on-going debate about the degree of localization versus itineracy in U intermetallics.

cond-mat.str-el↗

arXiv2023

Topotactically induced oxygen vacancy order in nickelate single crystals

The strong structure-property coupling in rare-earth nickelates has spurred the realization of new quantum phases in rapid succession. Recently, topotactic transformations have provided a new platform for the controlled creation of oxygen vacancies and, therewith, for the exploitation of such coupling in nickelates. Here, we report the emergence of oxygen vacancy ordering in Pr$_{0.92}$Ca$_{0.08}$NiO$_{2.75}$ single crystals obtained via a topotactic reduction of the perovskite phase Pr$_{0.92}$Ca$_{0.08}$NiO$_{3}$, using CaH$_2$ as the reducing agent. We unveil a brownmillerite-like ordering pattern of the vacancies by high-resolution scanning transmission electron microscopy, with Ni ions in alternating square-pyramidal and octahedral coordination along the pseudocubic [100] direction. Furthermore, we find that the crystal structure acquires a high level of internal strain, where wavelike modulations of polyhedral tilts and rotations accommodate the large distortions around the vacancy sites. Our results suggest that atomic-resolution electron microscopy is a powerful method to locally resolve unconventional crystal structures that result from the topotactic transformation of complex oxide materials.

cond-mat.mtrl-sci↗

arXiv2023

Resonant Inelastic X-ray Scattering from Electronic Excitations in $α$-RuCl$_3$ Nanolayers

We present Ru $L_3$-edge resonant inelastic x-ray scattering (RIXS) measurements of spin-orbit and d-d excitations in exfoliated nanolayers of the Kitaev spin-liquid candidate RuCl$_3$. Whereas the spin-orbit excitations are independent of thickness, we observe a pronounced red-shift and broadening of the d-d excitations in layers with thickness below $\sim$7 nm. Aided by model calculations, we attribute these effects to distortions of the RuCl$_6$ octahedra near the surface. Our study paves the way towards RIXS investigations of electronic excitations in various other 2D materials and heterostructures.

cond-mat.str-el↗

arXiv2023

Tracing the dynamics of superconducting order via transient third harmonic generation

Ultrafast optical control of quantum systems is an emerging field of physics. In particular, the possibility of light-driven superconductivity with ultrashort laser pulses has attracted much of attention. To identify non-equilibrium superconductivity, it is necessary to measure fingerprints of superconductivity on ultrafast timescales. Recently non-linear THz third harmonic generation (THG) was shown to directly probe the collective degrees of freedoms of the superconducting condensate including particularly the Higgs mode. Here we extend this idea to light-driven non-equilibrium states in superconducting La2-xSrxCuO4 establishing a protocol to access the transient superconducting (SC) order-parameter fluctuations. We perform an optical pump-THz-THG drive experiment and use a two-dimensional spectroscopy approach to disentangle the driven third-harmonic response of optically excited quasiparticles and the pure condensate response. In this way, 2D spectroscopy separately probes both the ultrafast pair breaking dynamics and transient pairing amplitude of the condensate.

cond-mat.supr-con↗

arXiv2023

Synthesis and physical properties of LaNiO$_2$ crystals

Infinite-layer (IL) nickelates are an emerging family of superconductors whose similarities and differences to cuprate superconductors are under intense debate. To date, the IL phase of nickelates can only be reached via topotactic oxygen reduction of the perovskite phase, using H$_2$ gas or reducing agents such as CaH$_2$. While the topotactic reduction method has been widely employed on thin film and polycrystalline powder samples, the reduction of La$_{1-x}$Ca$_x$NiO$_3$ single-crystals with lateral dimensions up to 150 $μ$m was achieved only recently, using an indirect contact method with CaH$_2$. Here we report the topotactic transformation of much larger LaNiO$_3$ crystals with lateral dimensions of more than one millimeter, via direct contact with CaH$_2$. We characterize the crystalline, magnetic, and electronic properties of the obtained IL LaNiO$_{2}$ crystals by powder and single-crystal x-ray diffraction (XRD), magnetometry, electrical transport, and x-ray photoelectron spectroscopy (XPS) measurements. The amount of incorporated topotactic hydrogen due to the reduction process is determined by a gas extraction method. In addition, we investigate the evolution of the lattice parameters under hydrostatic pressure up to 12 GPa, using high-resolution synchrotron XRD. Furthermore, we provide a direct comparison of several physical properties of the LaNiO$_{2}$ crystals to their powder and thin film counterparts.

cond-mat.supr-con↗

arXiv2022

Intense terahertz radiation via the transverse thermoelectric effect

Terahertz (THz) radiation is a powerful tool with widespread applications ranging from imaging, sensing, and broadband communications to spectroscopy and nonlinear control of materials. Future progress in THz technology depends on the development of efficient, structurally simple THz emitters that can be implemented in advanced miniaturized devices. Here we show how the natural electronic anisotropy of layered conducting transition metal oxides enables the generation of intense terahertz radiation via the transverse thermoelectric effect. In thin films grown on offcut substrates, femtosecond laser pulses generate ultrafast out-of-plane temperature gradients, which in turn launch in-plane thermoelectric currents, thus allowing efficient emission of the resulting THz field out of the film structure. We demonstrate this scheme in experiments on thin films of the layered metals PdCoO2 and La1.84Sr0.16CuO4, and present model calculations that elucidate the influence of the material parameters on the intensity and spectral characteristics of the emitted THz field. Due to its simplicity, the method opens up a promising avenue for the development of highly versatile THz sources and integrable emitter elements.

cond-mat.mtrl-sci↗

arXiv2022

Investigation of hydrogen incorporations in bulk infinite-layer nickelates

Infinite-layer (IL) nickelates are an emerging class of superconductors, where the Ni$^{1+}$ valence state in a square planar NiO$_2$ coordination can only be reached via topotactic reduction of the perovskite phase. However, this topotactic soft chemistry with hydrogenous reagents is still at a stage of rapid development, and there is a number of open issues, especially considering the possibility of hydrogen incorporation. Here we study the time dependence of the topotactic transformation of LaNiO$_3$ to LaNiO$_2$ for powder samples with x-ray diffraction and gas extraction techniques. While the hydrogen content of the powder increases with time, neutron diffraction shows no negative scattering of hydrogen in the LaNiO$_2$ crystal lattice. The extra hydrogen appears to be confined to grain boundaries or secondary-phase precipitates. The average crystal structure, and possibly also the physical properties, of the primary LaNiO$_2$ phase are therefore not noticeably affected by hydrogen residues created by the topotactic transformation.

cond-mat.str-el↗

arXiv2021

Topotactic transformation of single-crystals: from perovskite to infinite-layer nickelates

Topotactic transformations between related crystal structures are a powerful emerging route for the synthesis of novel quantum materials. Whereas most such "soft chemistry" experiments have been carried out on polycrystalline powders or thin films, the topotactic modification of single crystals -- the gold standard for physical property measurements on quantum materials -- has proven remarkably difficult. Here, we report the topotactic reduction of La$_{1-x}$Ca$_{x}$NiO$_3$ single-crystals to La$_{1-x}$Ca$_{x}$NiO$_{2+δ}$ using CaH$_2$ as the reducing agent. The transformation from the three-dimensional perovskite to the quasi-two-dimensional infinite-layer phase was thoroughly characterized by X-ray diffraction, electron microscopy, Raman spectroscopy, magnetometry, and electrical transport measurements. Our work demonstrates that the infinite-layer structure can be realized as a bulk phase in crystals with micrometer-sized single-domains. The electronic properties of these specimens resemble those of epitaxial thin films rather than powders with similar compositions.

cond-mat.supr-con↗

arXiv2021

Fano interference of the Higgs mode in cuprate high-Tc superconductors

Despite decades of search for the pairing boson in cuprate high-Tc superconductors, its identity still remains debated to date. For this reason, spectroscopic signatures of electron-boson interactions in cuprates have always been a center of attention. For example, the kinks in the quasiparticle dispersion observed by angle-resolved photoemission spectroscopy (ARPES) studies have motivated a decade-long investigation of electron-phonon as well as electron-paramagnon interactions in cuprates. On the other hand, the overlap between the charge-order correlations and the pseudogap in the cuprate phase diagram has also generated discussions about the potential link between them. In the present study, we provide a fresh perspective on these intertwined interactions using the novel approach of Higgs spectroscopy, i.e. an investigation of the amplitude oscillations of the superconducting order parameter driven by a terahertz radiation. Uniquely for cuprates, we observe a Fano interference of its dynamically driven Higgs mode with another collective mode, which we reveal to be charge density wave fluctuations from an extensive doping- and magnetic field-dependent study. This finding is further corroborated by a mean field model in which we describe the microscopic mechanism underlying the interaction between the two orders. Our work demonstrates Higgs spectroscopy as a novel and powerful technique for investigating intertwined orders and microscopic processes in unconventional superconductors.

cond-mat.supr-con↗