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Ke-Jin Zhou

Publications and source records attributed to Ke-Jin Zhou.

At least 19 recordsLinked to original sources

RIXS Identification of Optical Phonon-Spin Coupling Effects in CrSBr

Resonant inelastic x-ray scattering provides experimental signatures of spin-phonon coupling in CrSBr through temperature-dependent Cr $L$-edge spectra. Low-energy excitations are observed exclusively in the low-temperature antiferromagnetic phase as energy-loss features. A quasi-elastic peak at approximately 42 meV is observed under $π$-polarization. Density functional theory phonon-mode calculations identify these RIXS features as occurring within the same energy range as bond-bending optical phonon modes associated with distortions of the Cr--S--Cr network. The pronounced suppression of these low-energy excitations upon warming into the paramagnetic phase, together with their polarization dependence, the calculated phonon spectrum, and a spin-renormalized electron-phonon RIXS framework, indicates a strong interplay between magnetic correlations and lattice dynamics. While the loss features appear at energies characteristic of optical phonons, the significant overlap of the optical-phonon and magnon bands suggests that the temperature-dependent behavior should not be regarded as purely lattice-derived excitations. Instead, the room-temperature suppression of the low-energy RIXS peaks is explained in terms of a spin-phonon coupling effect on the $L$-edge electron-phonon RIXS mechanism. The interpretation is supported by the combined experimental observations, phonon calculations, and theoretical modeling, rather than by temperature contrast alone. These results support spin-phonon coupling as a plausible and consistent interpretation of the observed temperature-dependent RIXS response and demonstrate that magnetic order can strongly influence phonon-related spectral weight in the RIXS spectrum.

cond-mat.mtrl-sci

$3d_{z^2}$ orbital delocalization and magnetic collapse in superconducting (La,Pr)$_3$Ni$_2$O$_{7-δ}$ films

The recent discovery of Ruddlesden--Popper (RP) nickelate thin-film superconductors has opened a new frontier in unconventional superconductivity. Its realization requires both compressive epitaxial strain and highly oxidative growth conditions, yet the microscopic pathway from the parent phase to the superconducting phase remains elusive. Here, X-ray absorption spectra and resonant inelastic X-ray scattering are employed to track this evolution by independently tuning strain and oxygen content in (La,Pr)$_3$Ni$_2$O$_{7-δ}$ thin films. We uncover a remarkable two-step narrative. First, signatures of delocalization emerge in the same way upon two independent tunings: Spectral weight transfers from a ''Upper Hubbard''-like peak to the hole-like peak associated with O $2p_z$ state, and in parallel, the initially localized Ni $3d_{z^2}$ orbital becomes more itinerant followed by the broadening and weakening of $dd$ orbital excitations. Second, as itinerancy increases, long-range spin-density-wave (SDW) order is suppressed in both intensity and correlation length, indicating direct competition with superconductivity. Yet, short-range magnons persist: they become damped but their bandwidth stays unchanged. Our results paint a coherent picture that both strain and oxygenation drive the RP bilayer nickelates towards the superconducting instability, where the O $2p_z$ and Ni $3d_{z^2}$ orbitals become delocalized. Concomitantly, the long-range magnetic order loses coherence and gets suppressed. These findings establish an orbital-selective route to RP nickelate superconductivity, in which the delocalization of the $2p_z$ and $3d_{z^2}$ orbitals and the robust short-range magnons upon the melting of SDW order are prerequisites, providing strong constraints for theory and the roadmap for designing nickelate superconductors.

cond-mat.supr-con

Dissecting superconductivity in the Ruddlesden-Popper nickelates: The role of electron correlation and interlayer magnetic exchange

The discovery of superconductivity in the Ruddlesden-Popper (RP) nickelates has opened a new chapter in the search for high superconducting transition temperatures ($T_\mathrm{c}$) materials. A central and puzzling feature of this family is the wide variation in $T_\mathrm{c}$ despite their common NiO$_2$ building blocks, as highlighted by the recent observation of superconductivity at $\sim$ 30 K in trilayer $\mathrm{La_4Ni_3O_{10}}$, significantly lower than 80 K reported in bilayer $\mathrm{La_3Ni_2O_7}$. Understanding the factors that control $T_\mathrm{c}$ in this family is therefore of paramount importance. Here, we use resonant inelastic x-ray scattering (RIXS) to investigate the electronic and magnetic excitations of $\mathrm{La_4Ni_3O_{10}}$ in direct comparison with its bilayer counterpart. Our results reveal a markedly different landscape. $\mathrm{La_4Ni_3O_{10}}$ exhibits a more itinerant character, evidenced by broader Ni $dd$ orbital excitations and a strong Ni 3$d$ fluorescence continuum, suggesting weaker electronic correlations than in the bilayer. Despite this, well-defined collective spin excitations persist, including dispersive acoustic and optical magnon branches alongside an incommensurate spin density wave. Using linear spin wave theory, we extract the interlayer superexchange interaction ($J_z$) to be $\sim$ 22 meV, much smaller than that in $\mathrm{La_3Ni_2O_7}$. The weaker correlation and reduced interlayer exchange together provide a consistent explanation for the substantially lower $T_\mathrm{c}$ in the trilayer compound. Our findings establish interlayer magnetic coupling and electronic correlation as key parameters governing superconductivity in layered nickelates and offer critical constraints for understanding the pairing mechanism in this emerging family.

cond-mat.supr-con

X-ray magnetic circular dichroism evidence of intrinsic $d$-wave altermagnetism in rutile-structure NiF$_2$

We present the x-ray magnetic circular dichroism (XMCD) at the Ni $L_{2,3}$-edge as an evidence of the $d$-wave altermagnetism in rutile-structure NiF$_2$. Sizable XMCD signal is observed in excellent agreement with theoretical simulations. Owing to a considerable net magnetization due to spin canting, the XMCD spectrum consists of an altermagnetic signal as well as a non-negligible ferromagnetic contribution. We verify experimentally that the XMCD spectrum can be written as a sum of contributions from altermagnetism and weak ferromagnetism. Two experimental methods to isolate the ferromagnetic contribution are shown to yield essentially the same result. These are dependence of XMCD on applied magnetic fields below the Néel temperature and the XMCD measured in applied field above the Néel temperature. Our results demonstrate the utility of XMCD as a probe for altermagnetic materials with the coexisting weak ferromagnetism induced by the relativistic spin-orbit coupling.

cond-mat.str-el

Superconducting phase diagram of multi-layer square-planar nickelates

The discovery of superconductivity in square-planar nickelates has offered a rich materials platform to explore the origins of cuprate-like superconductivity. Experimental investigations however have largely been limited to the infinite-layer $R$NiO$_2$ ($R$=rare-earth) nickelates. Here, we construct a phase diagram of multi-layer square-planar Nd$_{n+1}$Ni$_n$O$_{2n+2}$ compounds and discover signatures of superconductivity for $n$ = 4 - 8. Upon decreasing the dimensionality $n$, the superconducting anisotropy evolves due to 4$f$ electron effects, and electronic structure characteristics approach cuprate-like behavior. Magnetic fluctuations persist from within the superconducting regime and into the over-doped, non-superconducting regime. Remarkably, the superconducting regime overlaps with that of chemically-doped infinite-layer nickelates, demonstrating underlying commonalities and distinct differences across varying structural realizations of square-planar nickelates. Our work establishes this layered template for creating new nickel-based superconductors.

cond-mat.supr-con

Impact of Electron Correlations on Infinite-Layer Cuprates and Nickelates

Optimization of unconventional superconductivity involves a balance of interaction strengths. Precise determination of correlation strength across different material families is therefore important. Here, we present a combined X-ray absorption spectroscopy (XAS) and resonant inelastic X-ray scattering (RIXS) study of infinite-layer PrNiO$_2$ and SrCuO$_2$ that enables fair comparison of their interaction strengths. For both compounds, we study the orbital and magnetic excitations and extract their dispersions along high-symmetry directions. Using a single-band Hubbard model and including higher-order exchange interactions, we derive the correlation factor $U/t$ for both compounds. A key finding is that despite a smaller Coulomb repulsion $U$, PrNiO$_2$ exhibits a correlation strength that is 20% stronger than that of its isostructural cuprate counterpart SrCuO$_2$. This indicates that a moderation of the correlation strength may further optimize superconductivity in nickelates.

cond-mat.supr-con

Systematic Mapping of Altermagnetic Magnons by Resonant Inelastic X-Ray Circular Dichroism

Altermagnets, a unique class of magnetic materials that combines features of both ferromagnets and antiferromagnets, have garnered attention for their potential in spintronics and magnonics. While the electronic properties of altermagnets have been well studied, characterizing their magnon excitations is essential for fully understanding their behavior and enabling practical device applications. In this work, we introduce a measurement protocol combining resonant inelastic X-ray scattering with circular polarization and azimuthal scanning to probe the chiral nature of the altermagnetic split magnon modes in CrSb. This approach circumvents the challenges posed by domain averaging in macroscopic samples, allowing for precise measurements of the polarization and energy of the magnons in individual antiferromagnetic domains. Our findings demonstrate a pronounced circular dichroism in the magnon peaks, with an azimuthal dependence that is consistent with the theoretical predictions and the $g$-wave symmetry. By establishing a reliable and accessible method for probing altermagnetic magnons, this work opens new avenues for fundamental studies of these collective excitations and for developing next-generation magnonic device applications.

cond-mat.str-el

The doping evolution of the charge density wave and charge density fluctuations in La$_{2-x}$Sr$_x$CuO$_4$

Cuprate superconductors show various collective charge correlations that are intimately connected with their electronic properties. In particular, charge order in the form of an incommensurate charge density wave (CDW) order with an in-plane wavevector $δ_{\text{CDW}} \approx $ 0.23--0.35~r.l.u. appears to be universally present. In addition to CDW, dynamic charge density fluctuations (CDF) are also present with wavevectors comparable to $δ_{\text{CDW}}$. CDFs are present up to $\sim300\;$K and have relatively short correlation lengths of $ξ\sim 20$\;Å. Here we use Cu-$L_3$ and O-$K$ resonant inelastic X-ray scattering (RIXS) to study the doping dependence of CDW and CDFs in La$_{2-x}$Sr$_x$CuO$_4$. We fit our data with (quasi)elastic peaks resulting from the CDW and up to four inelastic modes associated with oxygen phonons that can be strongly coupled to the CDFs. Our analysis allows us to separate the charge correlations into three components: the CDW with wavevector $δ_{4a-\text{CDW}} \approx 0.24$ and two CDF components with $δ_{4a-\text{CDF}} \approx 0.24$ and $δ_{3a-\text{CDF}} \approx 0.30$. We find that for $T \approx T_c$ the CDW coexists with the CDFs for dopings near $x=p \sim 1/8$. The $4a$-CDW disappears beyond $x=0.16$ and the $4a$-CDF beyond $x=0.19$, leaving only a weak $3a$-CDF at the highest doping studied, $x=0.22$. Our data suggest that low-energy charge fluctuations exist up to doping $x=0.19=p^{\star}$, where the pseudogap disappears, however, we find no evidence that they are associated with a quantum critical point.

cond-mat.supr-con

Persistent paramagnons in high-temperature infinite-layer nickelate superconductors

The recent discovery of high-temperature superconductivity in hole-doped SmNiO$_2$, exhibiting the record-high transition temperature $T_c$ among infinite-layer (IL) nickelates, has opened a new avenue for exploring design principles of superconductivity. Experimentally determining the electronic structure and magnetic interactions in this new system is crucial to elucidating the mechanism behind the enhanced superconductivity. Here, we report a Ni $L$-edge resonant inelastic x-ray scattering (RIXS) study of superconducting Sm-based IL nickelate thin films Sm$_{1-x-y-z}$Eu$_x$Ca$_y$Sr$_z$NiO$_2$ (SECS). Dispersive paramagnonic excitations are observed in both optimally and overdoped SECS samples, supporting a spin-fluctuation-mediated pairing scenario. However, despite the two-fold enhancement of $T_c$ in the Sm-based nickelates compared to their Pr-based counterparts, the effective exchange coupling strength is reduced by approximately $20\%$. This behavior contrasts with hole-doped cuprates, where magnetic interactions correlate positively with $T_c$, highlighting essential differences in their superconducting mechanisms.

cond-mat.supr-con

Probing d-wave superconducting gap of high-$T_\mathrm{c}$ cuprate $\mathrm{Bi}_2\mathrm{Sr}_2\mathrm{Ca}_2\mathrm{Cu}_3\mathrm{O}_{10+δ}$ by resonant inelastic X-ray scattering

The superconducting gap is a characteristic feature of high-T$_c$ superconductors and provides crucial information on the pairing mechanism underlying high-temperature superconductivity. Here, we employ high-resolution resonant inelastic X-ray scattering (RIXS) at the Cu $L_3$-edge to investigate the superconducting gap in the overdoped cuprate $\mathrm{Bi}_2\mathrm{Sr}_2\mathrm{Ca}_2\mathrm{Cu}_3\mathrm{O}_{10+δ}$ ($T_\mathrm{c}$ = 107 K). By analyzing antisymmetrized, temperature-dependent RIXS spectra over a range of in-plane momentum transfers, we observe a clear suppression of low-energy spectral weight below T$_c$, indicative of superconducting gap formation. This suppression is most pronounced at small momentum transfers ($|\boldsymbol{q}_\parallel| \leq 0.18$ r.l.u.) and corresponds to a gap size of approximately 2$Δ_0 \sim$ 130 meV. Comparison with theoretical calculations of the momentum-dependent charge susceptibility supports a d-wave symmetry of the superconducting gap, while an isotropic s-wave gap fails to reproduce key experimental features. These findings establish RIXS as a powerful, bulk-sensitive probe of superconducting gap symmetry and highlight its utility for studying materials beyond the reach of surface-sensitive techniques such as ARPES and STM.

cond-mat.supr-con

Unconventional polaronic ground state in superconducting LiTi$_2$O$_4$

Geometrically frustrated lattices can display a range of correlated phenomena, ranging from spin frustration and charge order to dispersionless flat bands due to quantum interference. One particularly compelling family of such materials is the half-valence spinel Li$B_2$O$_4$ materials. On the $B$-site frustrated pyrochlore sublattice, the interplay of correlated metallic behavior and charge frustration leads to a superconducting state in LiTi$_2$O$_4$ and heavy fermion behavior in LiV$_2$O$_4$. To date, however, LiTi$_2$O$_4$ has primarily been understood as a conventional BCS superconductor despite a lattice structure that could host more exotic groundstates. Here, we present a multimodal investigation of LiTi$_2$O$_4$, combining ARPES, RIXS, proximate magnetic probes, and ab-initio many-body theoretical calculations. Our data reveals a novel mobile polaronic ground state with spectroscopic signatures that underlie co-dominant electron-phonon coupling and electron-electron correlations also found in the lightly doped cuprates. The cooperation between the two interaction scales distinguishes LiTi$_2$O$_4$ from other superconducting titanates, suggesting an unconventional origin to superconductivity in LiTi$_2$O$_4$. Our work deepens our understanding of the rare interplay of electron-electron correlations and electron-phonon coupling in unconventional superconducting systems. In particular, our work identifies the geometrically frustrated, mixed-valence spinel family as an under-explored platform for discovering unconventional, correlated ground states.

cond-mat.supr-con

Dominant apical-oxygen electron-phonon coupling in HgBa$_2$Ca$_2$Cu$_3$O$_{8+δ}$

How electron-phonon interactions influence high-temperature superconductivity in cuprates remains contested, and their role outside the CuO$_2$ planes has been largely overlooked. The most conspicuous evidence for such coupling is the ubiquitous 70-meV dispersion kink seen by photoemission, yet its microscopic origin is still debated. Here we use oxygen-$K$-edge resonant inelastic X-ray scattering (RIXS) to probe the trilayer cuprate HgBa$_2$Ca$_2$Cu$_3$O$_{8+δ}$ (Hg1223). When both incident photon energy and polarization are tuned to the apical-oxygen $1s\!\rightarrow\!2p_z$ transition, the RIXS spectra exhibit a ladder of at least ten phonon overtones, evenly spaced by 70 meV, whose intensities follow a Franck-Condon envelope, signalling exceptionally strong electron-phonon coupling. Quantitative modelling that incorporates core-hole lifetime evaluation yields an apical-phonon coupling energy of 0.25(1) eV, significantly larger than that of the planar stretching mode. Such a coupling strength offers a strong contender for explaining the universal 70-meV kink and suggests that the dominant electron-phonon channel resides outside the CuO$_2$ planes. By elevating inter-layer lattice dynamics from a peripheral factor to a central actor, our results provide a fresh starting point for theories seeking to reconcile strong correlations, lattice dynamics and high-temperature superconductivity.

cond-mat.supr-con

Magnetic excitations in Nd$_{n+1}$Ni$_{n}$O$_{3n+1}$ Ruddlesden-Popper nickelates observed via resonant inelastic x-ray scattering

Magnetic interactions are thought to play a key role in the properties of many unconventional superconductors, including cuprates, iron pnictides, and square-planar nickelates. Superconductivity was also recently observed in the bilayer and trilayer Ruddlesden-Popper nickelates, whose electronic structure is expected to differ from that of cuprates and square-planar nickelates. Here we study how electronic structure and magnetic interactions evolve with the number of layers, $n$, in thin film Ruddlesden-Popper nickelates Nd$_{n+1}$Ni$_{n}$O$_{3n+1}$ with $n=1,\:3$, and 5 using resonant inelastic x-ray scattering (RIXS). The RIXS spectra are consistent with a high-spin $|3d^8 \underline{L} \rangle$ electronic configuration, resembling that of La$_{2-x}$Sr$_x$NiO$_4$ and the parent perovskite, NdNiO$_3$. The magnetic excitations soften to lower energy in the structurally self-doped, higher-$n$ films. Our observations confirm that structural tuning is an effective route for altering electronic properties, such as magnetic superexchange, in this prominent family of materials.

cond-mat.str-el

Chiral phonons in polar LiNbO3

Quasiparticles describe collective excitations in many-body systems, and their symmetry classification is of fundamental importance because they govern physical processes on various timescales, e.g., excited states, transport phenomena, and phase transitions. Recent studies have revealed that quasiparticles can possess chirality and that this degree of freedom leads to various important phenomena. Among them, chiral phonons have recently attracted significant interest because of their intrinsic magnetism, which non-trivially bridges the spin system and the lattice. Here, we directly prove the presence of chiral phonons in a prototypical polar crystal LiNbO3. Our demonstration adds a polar crystal in the showcase of materials hosting chiral phonons and, furthermore, creates a substantial potential in chiral phononics because of its expected in-situ switchable phonon chirality and associated control of phonon angular momentum.

cond-mat.str-el

Observation of collective charge excitations in a cuprate superconductor

Emergent symmetry breakings in condensed matter systems are often intimately linked to collective excitations. For example, the intertwined spin-charge stripe order in cuprate superconductors is associated with spin and charge excitations. While the collective behavior of spin excitations is well established, the nature of charge excitations remains to be understood. Here we present a high-resolution resonant inelastic x-ray scattering (RIXS) study of charge excitations in the stripe-ordered cuprate La$_{1.675}$Eu$_{0.2}$Sr$_{0.125}$CuO$_4$. The RIXS spectra consist of both charge and phonon excitations around the charge ordering wave vector. By modeling the momentum-dependent phonon intensity, the charge-excitation spectral weight is extracted for a wide range of energy. As such, we reveal the highly dispersive nature of the charge excitations, with an energy scale comparable to the spin excitations. Since charge order and superconductivity in cuprates are possibly driven by the same electronic correlations, determining the interaction strength underlying charge order is essential to establishing a comprehensive microscopic model of high-temperature superconductivity.

cond-mat.supr-con

Decoupling of Static and Dynamic Charge Correlations revealed by Uniaxial Strain in a Cuprate Superconductor

We use uniaxial strain in combination with ultra-high-resolution Resonant Inelastic X-ray Scattering (RIXS) at the oxygen K- and copper L3-edges to study the excitations stemming from the charge ordering wave vector in La1.875Sr0.125CuO4. By detwinning stripe ordering, we demonstrate that the optical phonon anomalies do not show any stripe anisotropy. The low-energy charge excitations also retain an in-plane four-fold symmetry. As such, we find that both phonon and charge excitations are decoupled entirely from the strength of static charge ordering. The almost isotropic character of charge excitations is indicative of a quantum critical behaviour and remains a possible source for the strange metal properties found in the normal state of cuprate superconductors.

cond-mat.str-el

Circular Dichroism in Resonant Inelastic X-ray Scattering: Probing Altermagnetic Domains in MnTe

X-ray magnetic circular dichroism provides a means to identify ferromagnetic, chiral, and altermagnetic orders via their time-reversal-symmetry ($\mathcal{T}$) breaking. However, differentiating magnetic domains related by crystallographic symmetries remains a technical challenge. Here we reveal a circular dichroism (CD) in the resonant inelastic x-ray scattering (RIXS) spectra from the altermagnetic MnTe. The azimuthal dependence of the RIXS-CD intensity of the magnon excitations indicates a dominant occupation of a single altermagnetic domain. The RIXS-CD in our scattering geometry is ascribed to the mirror-symmetry breaking associated with the $\mathcal{T}$-broken altermagnetic order. Our results establish RIXS-CD as a domain-sensitive probe of elementary excitations in quantum materials.

cond-mat.str-el

Circular dichroism in resonant inelastic x-ray scattering from birefringence in CuO

Resonant inelastic x-ray scattering (RIXS) has become a prominent technique to study quasiparticle excitations. With advances in polarization analysis capabilities at different facilities, RIXS offers exceptional potential for investigating symmetry-broken quasiparticles like chiral phonons and magnons. At optical wavelengths birefringence can severely affect polarization states in low-symmetry systems. Here we show its importance for soft x-ray resonances. Given the growing interest in Circular Dichroism (CD) in RIXS, it is important to evaluate how birefringence may affect the RIXS spectra of anisotropic systems. We investigate CuO, a well-known anisotropic material, using Cu $L_3$-edge RIXS and detect significant CD in both magnetic and orbital excitations in the collinear antiferromagnetic phase. We demonstrate that the CD can be modeled by a proper treatment of RIXS scattering amplitudes derived from single-ion calculations with birefringence. Recognizing these effects is crucial for unambiguous identification of subtle dichroic effects induced by symmetry-broken quasiparticles. Furthermore, the combined sensitivity of RIXS and birefringence to local symmetry presents an opportunity to study microscopic changes driven by external perturbations.

cond-mat.mtrl-sci