arXiv subjects

B. Keimer

Publications and source records attributed to B. Keimer.

At least 19 recordsLinked to original sources

arXiv2026

Separating the Density Wave Phase from Zero-Resistance Superconductivity in La$_4$Ni$_3$O$_{10}$

Identifying the key ingredients for superconductivity under pressure in the Ruddlesden-Popper nickelates remains a formidable challenge, due to a complex interplay between structural variations, oxygen content and location, electronically ordered phases, and the need for high pressures to reach the superconducting phase. To disentangle these complex inter-dependencies, here we study a series of clean single crystals of trilayer La$_4$Ni$_3$O$_{10}$. We discover that enhanced biaxial, compressive pressures induce a zero-resistance state at a 60\% lower pressure compared to previous reports. At the same time, we completely separate the low-pressure density wave phase from superconductivity, effectively ruling out that soft, quantum critical fluctuations of the density wave order parameter act as the pairing glue in this system. Our results establish biaxial, in-plane pressures as a powerful tool for promoting superconductivity in nickelates, unifying the required pressure scales for superconductivity in different Ruddlesden-Popper structures, and providing a connection to the recently discovered thin film samples.

cond-mat.supr-con↗

arXiv2026

Unambiguous determination of the THz conductivity in driven YBa$_2$Cu$_3$O$_{6+x}$

Mid-infrared pump, THz probe experiments in YBa$_2$Cu$_3$O$_{6+x}$ yield evidence of a high-temperature transient state of the material with the optical properties of a superconductor. However, there are ambiguities in the extracted transient c-axis THz optical properties, primarily resulting from the sublinear growth of the THz response with increasing mid-infrared pump fluence. It was proposed that this effect may be related to saturation of the material's response, which would then perturb its spatial profile and lead one to overestimate the induced change in the transient optical properties. Yet, sublinear growth of the signal could also arise from other effects unrelated to saturation, for example from a change in reflectivity or deposition depth for the pump pulses. Here, we remove this ambiguity by experimentally measuring the fluence-dependent complex optical constants at the 15-20 THz frequencies of the pump. We show that the observed sublinear growth is to be attributed in large part to the enhanced reflection and reduced penetration depth of the pump field at high fluences. When taking into account these findings, we confirm the original interpretation of a light-induced superconducting state both qualitatively and quantitatively.

cond-mat.supr-con↗

arXiv2026

Coherence and pairing enhancement in a trilayer cuprate with layer-selective charge order

Trilayer cuprates hold the record for the highest superconducting critical temperatures ($T_{\text{c}}$), yet the underlying mechanism remains elusive. Using time- and angle-resolved photoemission spectroscopy (tr-ARPES), we uncover a striking interplay between charge order, superconducting gap magnitude, and quasiparticle coherence in Bi$_2$Sr$_2$Ca$_2$Cu$_3$O$_{10+δ}$ (Bi2223). We present ARPES-based evidence of charge order on the inner CuO$_2$ plane -- as confirmed via resonant x-ray scattering (RXS) -- and show that the same inner plane hosts a large superconducting gap matching its doping, firmly establishing it as underdoped. Despite its underdoped nature, the inner plane also exhibits an exceptional degree of quasiparticle coherence; suppressing charge-order fluctuations further enhances this, making it comparable to that of the overdoped outer planes at elevated electronic temperatures. At the same time, on the overdoped outer planes we find larger superconducting gaps than what is seen on comparably doped single and bilayer cuprates, indicating an unexpected and simultaneous enhancement of both coherence and pairing interactions in Bi2223. These findings, supported by complementary single- and three-layer Hubbard model calculations, reveal a unique interlayer mechanism in which both pairing strength and phase coherence are optimized when interfacing planes with distinct hole concentrations, providing new microscopic insight into the record $T_{\text{c}}$ of Bi2223.

cond-mat.str-el↗

arXiv2026

Multiorbital character of the density wave in trilayer nickelate superconductors

Ruddlesden-Popper nickelates exhibit high-temperature superconductivity closely intertwined with charge and spin density waves. However, fundamental questions persist regarding the interplay between the associated density wave (DW) fluctuations and superconductivity, as well as the orbital character and symmetry underlying the DW instabilities. Here we utilize polarized Raman scattering to investigate the phononic and electronic Raman responses of the trilayer nickelate La$_4$Ni$_3$O$_{10}$ across its concomitant charge and spin density wave transitions. In addition to distinct phonon anomalies occurring below the transition temperature, we observe a depletion of continuum spectral weight up to 114 meV and a pronounced peak centered at this energy. By combining momentum-selective information from polarized electronic Raman scattering with Raman-response model calculations based on a multiorbital Raman vertex in a reconstructed two-orbital DW state involving both Ni-3$d_{x^2 - y^2}$ and Ni-3$d_{z^2}$ orbitals, we identify 114 meV as the energy scale $2Δ_\mathrm{DW}$ of the DW gap, characterized by incoherent opening and non-mean-field behavior. Furthermore, the model calculations reveal that the corresponding $2Δ_\mathrm{DW}$ peak has a multiorbital origin, requiring both orbital contributions and their mixing beyond single-orbital projections, thus shedding light on the nature of the DW instabilities in La$_4$Ni$_3$O$_{10}$.

cond-mat.str-el↗

arXiv2026

Magnetic circular dichroism of THz modes and selection rules of Raman-active optical phonons in the polar altermagnet candidate \ce{Mn2Mo3O8}

We investigated the magnetic and vibrational excitations in the collinear altermagnet candidate \ce{Mn2Mo3O8} by temperature dependent Raman scattering and magneto-optical THz time-domain transmission spectroscopy. By comparison to \textit{ab initio} calculations accurately capturing the eigenfrequencies of the vibrational eigenmodes, we identify all optical phonons, including the lowest-lying Raman modes of $A_1$ and $E_2$ type, which had remained elusive in a previous Raman study. Moreover, we compare the selection rules for optically active phonons in the paramagnetic and the magnetically ordered phases of \ce{Mn2Mo3O8} and analyze the Raman selection rules with respect to pseudo-angular momentum conservation. No evidence of the expected splitting of the degenerate paramagnetic $E_2$ optical phonons into modes with circular polarization upon magnetic ordering could be resolved, likely due to weak spin-orbit coupling typical for Mn$^{2+}$. In contrast, we observe strong magnetic circular dichroism at a broad THz excitation band, emerging in the magnetically ordered state. This band, potentially originating from two-magnon excitations, is only electric-dipole active and features a field-dependent two-component fine structure. Its magnetic circular dichroism vanishes above the spin-flop transition at 4~T.

cond-mat.str-el↗

arXiv2026

High temperature transitions in Ruddlesden-Popper nickelates La$_{n+1}$Ni$_{n}$O$_{3n+1}$

The discovery of superconductivity at $15\,\mathrm{K}$ in the infinite-layer nickelate $(\mathrm{Nd},\mathrm{Sr})\mathrm{NiO}_2$, followed by superconductivity at $80\,\mathrm{K}$ in the Ruddlesden--Popper phase $\mathrm{La}_3\mathrm{Ni}_2\mathrm{O}_7$, has ushered in a new era of nickelate research. Despite this progress, large discrepancies between reports exist. Here, we investigate the complete series of bulk-stable $\mathrm{La}_{n+1}\mathrm{Ni}_n\mathrm{O}_{3n+1}$ compounds using a comprehensive set of experimental techniques, including PXRD, single-crystal XRD, electron microscopy, heat capacity, differential scanning calorimetry, magnetic susceptibility, and transport measurements, over a broad temperature range from $2$ to $1000\,\mathrm{K}$. By studying high-quality single crystals, we identify a previously underappreciated high-temperature phase transition in Ruddlesden--Popper nickelates $\mathrm{La}_{n+1}\mathrm{Ni}_n\mathrm{O}_{3n+1}$ distinct from the one going to a tetragonal phase.

cond-mat.supr-con↗

arXiv2026

Non-magnetic ground state in A$_2$WCl$_6$ (A = Cs, Rb, K): A face-centered cubic system of spin-orbit-entangled $J$ = 2 states

Heavy transition metal compounds with strong spin-orbit coupling appeared as a platform for $d$-electron multipolar physics. We report the electronic, magnetic, and structural properties of antifluorite-type tungsten chloride A$_2$WCl$_6$ (A = Cs, Rb, and K), comprising a face-centered cubic lattice of W$^{4+}$ ions. The 5$d^2$ configuration of W$^{4+}$ ions in a cubic environment yields a spin-orbit-entangled $J$ = 2 state, which has been discussed to give rise to multipolar ordering such as charge quadrupolar or magnetic octupolar ordering. We found that K$_2$WCl$_6$ undergoes a cubic-to-tetragonal structural transition which lifts the degeneracy of the $J$ = 2 state, leading to a non-magnetic singlet ground state. By contrast, Rb$_2$WCl$_6$ and Cs$_2$WCl$_6$ show no signs of phase transition and remain non-magnetic down to the lowest temperature measured. At low temperatures, signatures of weak structural anomalies were revealed, which may point to the presence of local distortions of the WCl$_6$ octahedra. We argue that the subtle structural distortion arises from the local quadrupolar component of the $J$ = 2 state but the frustrated quadrupolar interaction, together with chemical disorder, inhibits the formation of long-range quadrupolar ordering.

cond-mat.str-el↗

arXiv2026

Three-dimensional zigzag correlations in the van der Waals Kitaev magnet RuBr$_3$

Ruthenium trihalides Ru$X_3$ ($X$ = Cl, Br, I) provide a tunable platform for Kitaev magnetism in two-dimensional van der Waals materials. Despite their similar crystal structures and zigzag antiferromagnetic order, RuBr$_3$ exhibits a higher Néel temperature ($T_N$) than RuCl$_3$, suggesting their distinct proximity to the Kitaev quantum spin liquid phase. Using Ru $L_3$-edge resonant x-ray scattering, we show that, while the long-range zigzag order in RuBr$_3$ disappears at $T_N$, the zigzag correlations that persist well above $T_N$ show a pronounced spectral weight redistribution along the interlayer direction. These results suggest that the enhanced interlayer magnetic interactions driven by the extended Br 4$p$ orbitals stabilize three-dimensional zigzag correlations in RuBr$_3$.

cond-mat.str-el↗

arXiv2026

From perovskite to infinite-layer nickelates: hole concentration from x-ray absorption

The difficulty of determining cation concentrations and oxygen stoichiometry in infinite-layer nickelate thin films has so far prevented clear experimental identification of the nickel electron configuration in the superconducting phase. We used soft x-ray absorption spectroscopy to study the successive changes in PrNiO$_x$ thin films at various intermediate stages of topotactic reduction with $x=2-3$. By comparing the Ni-$L$ edge spectra to single and double cluster ligand-field calculations, we find that none of our samples exhibit a pure $d^9$ configuration. Our quantitative analysis using the charge sum rule shows that even when films are maximally reduced, the averaged number of nickel $3d$ holes is 1.35. Superconducting samples have even higher values, calling into question the previously assumed limit of hole doping. Concomitant changes in the oxygen $K$-edge absorption spectra upon reduction indicate the presence of oxygen $2p$ holes, even in the most reduced films. Overall, our results suggest a complex interplay of hole doping mechanisms resulting from self-doping effects and oxygen non-stoichiometry.

cond-mat.supr-con↗

arXiv2026

Signatures of three-dimensional photo-induced superconductivity in YBa$_2$Cu$_3$O$_{6.48}$

Optical excitation of large-amplitude apical oxygen phonon oscillations has been shown to renormalize the electronic properties of YBa$_2$Cu$_3$O$_{6+x}$, inducing a superconducting-like optical response above equilibrium $T_C$. All of the evidence collected so far has been based on the changes of the THz frequency $c$-axis response. In these measurements, the capacitive interlayer coupling was seen to transform into a superconducting-like inductive response. This assignment was strengthened by recent measurements of ultrafast magnetic field expulsion. Here, we report an experimental determination of the transient in-plane optical properties, which has so far been elusive due to the high equilibrium reflectivity and the need to evaluate minute changes in the optical response. We report the appearance of a photo-induced in-plane optical gap $2Δ\simeq30$ cm$^{-1}$ and a divergent imaginary conductivity, both consistent with photo-induced superconductivity. A global fit to these data suggests that in- and out-of-plane electronic properties never completely equilibrate during the dynamics.

cond-mat.supr-con↗

arXiv2025

Hybridization of lattice and charge order excitations in a superconducting cuprate

The ubiquitous tendency of superconducting cuprates to form charge density waves (CDWs) has reignited interest in the nature of their electron-phonon interaction and its role in shaping their phase diagrams. While pronounced dispersion anomalies were reported in several phonon branches, their precise connection to charge order and superconductivity remains unresolved. Here, using high-resolution inelastic x-ray scattering under low temperature and high magnetic field, we uncover a striking phonon renormalization in YBa$_2$Cu$_3$O$_{6+x}$. It appears along a reciprocal space trajectory connecting the wave vectors of a short-range 2D-CDW, emerging above the superconducting transition, and a long-range 3D-CDW, appearing only when superconductivity is strongly suppressed. The spectral changes are strongest around the wave vector of the 3D-CDW despite the fact that it is absent in our experimental conditions. Our findings challenge conventional phonon self-energy renormalization models, instead support a scenario in which low-energy phonons hybridize with dispersive CDW excitations and provide insights into the interplay between lattice vibrations and electronic correlations in high-temperature superconductors.

cond-mat.supr-con↗

arXiv2025

Enhanced coherent terahertz emission from critical superconducting fluctuations in YBa$_2$Cu$_3$O$_{6.6}$

Coherent terahertz (THz) emission is emerging as a powerful new tool to probe symmetry breakings in quantum materials. This method relies on second order optical nonlinearities and is complementary to second harmonic generation spectroscopy. Here, we report coherent THz emission from Josephson plasmons in underdoped YBa$_2$Cu$_3$O$_{6+x}$, and find that the amplitude of the emitted field increases dramatically close to the superconducting transition temperature, $T_C$. We show theoretically how emission is enhanced by critical superconducting fluctuations, a nonlinear analogue of critical opalescence. This observation is expected to be of general importance for the study of many thermal and quantum phase transitions.

cond-mat.supr-con↗

arXiv2025

Uniaxial strain tuning of polar lattice vibrations in KTaO$_3$ and SrTiO$_3$

The interplay of electronic and structural degrees of freedom is a prominent feature of many quantum materials and of particular interest in systems with strong ferroelectric fluctuations, such as SrTiO$_3$ (STO) and KTaO$_3$ (KTO). Both materials are close to a ferroelectric transition, but despite six decades of extensive research, pivotal questions regarding the nature of this transition and of the associated fluctuations remain debated. Here we combine inelastic neutron scattering, Raman spectroscopy, and ab initio calculations to study the evolution of soft polar phonons across the strain-induced ferroelectric transition in STO and KTO. We find that the modes remain underdamped and at nonzero energy, consistent with a first-order quantum phase transition. We also reveal a strong violation of the well-known Lyddane-Sachs-Teller relation between the phonon energies and static dielectric permittivities in insulating KTO and STO, which is not captured by ab initio calculations and points to the presence of slow mesoscale fluctuations induced by long-range interactions. In metallic STO, we uncover a first-order transition at a remarkably low critical stress, in qualitative agreement with recent theoretical predictions. The present work resolves several long-standing questions pertaining to the model systems STO and KTO and is relevant to numerous other materials with soft polar phonons.

cond-mat.mtrl-sci↗

arXiv2025

Evolution of spin excitations in superconducting La$_{2-x}$Ca$_{x}$CuO$_{4-δ}$ from the underdoped to the heavily overdoped regime

We investigate high-energy spin excitations in hole-doped La$_{2-x}$Ca$_{x}$CuO$_{4-δ}$ films across a broad Ca doping range $x = 0.05-0.50$ using resonant inelastic x-ray scattering (RIXS). Polarization analysis and incident-photon energy detuning measurements confirm the persistence of collective paramagnon excitations up to $x = 0.50$. Consistent with previous studies on other cuprate families, we observe a pronounced crossover near $x = 0.15$, where paramagnon spectral weight is transferred to incoherent spin-flip excitations associated with the particle-hole continuum. The overall behavior of paramagnons in LCCO resembles that in other hole-doped cuprates and appears insensitive to the persistence of superconductivity at high doping levels in LCCO - up to at least $x = 0.50$, as demonstrated in prior work. These findings support the view that high-energy magnetic excitations probed by RIXS are not a major contributor to superconducting pairing, in line with theories of spin-fluctuation mediated superconductivity.

cond-mat.supr-con↗

arXiv2025

Coincident onset of charge order and pseudogap in a homogeneous high-temperature superconductor

Understanding high-temperature superconductivity in cuprates requires knowledge of the metallic phase it evolves from, particularly the pseudogap profoundly affecting the electronic properties at low carrier densities. A key question is the influence of chemical disorder, which is ubiquitous but exceedingly difficult to model. Using resonant x-ray scattering, we identified two-dimensional charge order in stoichiometric YBa$_2$Cu$_4$O$_8$ ($T_c$ = 80 K), which is nearly free of chemical disorder. The charge order amplitude shows a concave temperature dependence and vanishes sharply at $T^*$ = 200 K, the onset of a prominent pseudogap previously determined by spectroscopy, suggesting a causal link between these phenomena. The gradual onset of charge order in other cuprates is thus likely attributable to an inhomogeneous distribution of charge ordering temperatures due to disorder induced by chemical substitution. The relationship between the pseudogap and the disorder-induced gradual freeze-out of charge carriers remains a central issue in research on high-$T_c$ superconductors.

cond-mat.supr-con↗

arXiv2025

Resonant x-ray scattering study of charge-density wave correlations in YBa$_{2}$Cu$_{3}$O$_{6+x}$ under uniaxial stress

We report a comprehensive study of the uniaxial stress response of charge-density-wave (CDW) correlations in detwinned single crystals of the high temperature superconductor YBa$_2$Cu$_3$O$_{6+x}$ (YBCO$_{6+x}$) with $0.40 \leq x \leq 0.93$ (hole-doping levels $0.072 \leq p \leq 0.168$) by means of Cu $L_3$-edge resonant energy-integrated x-ray scattering (REXS). We show that the influence of uniaxial stress is strongly doping dependent: the quasi-two-dimensional CDW is enhanced by in-plane uniaxial stress in a wide hole doping range ($0.45 \leq x \leq 0.80$), but only barely affected in the most underdoped and optimally doped samples ($x = 0.40$ and 0.93), where the CDW correlation length is minimal. A stress-induced three-dimensionally long-range ordered (3D) CDW was observed only in YBCO$_{6.50}$ and YBCO$_{6.67}$. The temperature dependence of the 3D CDW clearly indicates a strong competition with superconductivity. Based on the systematic strain-, doping-, and temperature-dependent REXS measurements reported here, we discuss the relationship between charge order and superconductivity in YBCO$_{6+x}$ and other cuprates.

cond-mat.supr-con↗

arXiv2025

Magnetic ground state of the dimer-based hexagonal perovskite Ba$_{3}$ZnRu$_{2}$O$_{9}$

We investigate the magnetic ground state of single crystals of the ruthenium-dimer-based hexagonal perovskite Ba$_{3}$ZnRu$_{2}$O$_{9}$ using magnetic susceptibility and resonant inelastic x-ray scattering (RIXS) measurements. While a previous study on powder samples exhibited intriguing magnetic behavior, questions about whether the spin state within a Ru$_{2}$O$_{9}$ dimer is a conventional $S = 3/2$ dimer or an orbital-selective $S = 1$ dimer were raised. The RIXS spectra reveal magnetic excitations from Hund's intraionic multiplet and intradimer spin-triplet transitions. The observed transition energies of the Hund's intraionic multiplets align with the $S=3/2$ ground state, contrasting with the theoretically proposed orbital-selective $S=1$ dimer state. High-temperature magnetic susceptibility analysis confirms the realization of the spin $S=3/2$ dimer state, and the extracted intradimer coupling is consistent with the spin-triplet transition energy observed in the RIXS spectra. These results highlights the ability of "spectroscopic fingerprinting" by RIXS to determine the magnetic ground states of complex materials.

cond-mat.str-el↗

arXiv2025

Signatures of two gaps in the spin susceptibility of a cuprate superconductor

A major obstacle to understanding high-Tc cuprates is that superconductivity precludes observing normal-state properties at low temperatures. One prime example is the normal-state spin susceptibility \c{hi}spin: although its decrease upon cooling far above Tc typifies pseudogap behavior, its behavior at low temperatures is generally unknown. Here, our measurements in high magnetic fields expose \c{hi}spin of YBa2Cu3Oy down to low temperatures. Even though superconductivity is suppressed by the field, we uncover two thermally-activated contributions alongside a residual \c{hi}spin(T=0) due to gapless excitations. We relate these two distinct gaps to short-range charge-density waves and to the formation of singlets as in certain quantum spin systems. Both phenomena thus contribute to the pseudogap at low temperature, supplementing short-lived antiferromagnetism that initiates pseudogap behavior at high temperatures. We therefore propose that the pseudogap ought to be regarded as a composite property and that, when not undergoing spin-stripe ordering, underdoped cuprates tend to form short-ranged spin singlets.

cond-mat.supr-con↗