arXiv subjects

Ke-Jun Xu

Publications and source records attributed to Ke-Jun Xu.

13 recordsLinked to original sources

arXiv2026

Selective coupling of high-order phonons in La2-xSrxCuO4

In crystals and molecules with strong coupling between the charge carriers and atomic vibrations, high order harmonics of the vibrational excitations can be observed with intensity following the Franck-Condon envelope. Here, we uncover a new regime of electron-phonon coupling in La2-xSrxCuO4 using resonant inelastic X-ray scattering. In the undoped compound, we find sharp peaks at approximately 85$\pm$5 meV, 180$\pm$7 meV, and 330$\pm$5 meV with no observable dispersion, and an absence of appreciable intensity from other modes observed in Raman spectroscopy in this energy range. The 180 meV and 330 meV excitations have energies approximately consistent with two-phonon and four-phonon in-plane Cu-O bond stretching mode, suggesting that the resonantly excited valence electrons strongly couple to this mode. These excitations exhibit significant doping dependence, eventually becoming unresolvable at 10% hole doping, where the low energy charge excitations are dominated by dispersive plasmons. The observation of selective coupling to even-ordered phonons and stark contrast with the Raman spectra indicate anomalous electron-phonon coupling beyond the Franck-Condon picture. One intriguing possibility is the existence of locally paired quasiparticles in insulating cuprates.

cond-mat.str-el↗

arXiv2026

Spectroscopic evidence for a molecular orbital Kondo insulator

A Kondo insulator (KI) is a prototypical example of a highly entangled phase of matter, where many-body interactions between local moments and delocalized electrons engender the non-magnetic insulating ground state. Conventionally, the local moments arise from atomic multiplet states with a narrow bandwidth, limiting Kondo coherence to low temperatures. Here, we realize a new paradigm for constructing the KI state with hybridized molecular orbitals in FeSb2. Resonant inelastic X-ray scattering (RIXS) at the Fe L-edge reveals distinct signatures of band-like continuum states and localized states. Comparisons with first-principles calculations establish a mixed-configuration ground state with hybridized Fe d-Sb p molecular orbitals as basis states. By systematically investigating the RIXS momentum, temperature, and doping dependences, we find propagating collective modes commensurate with many-body charge and spin excitations. Our results pave the way for understanding the emerging class of unconventional d electron insulators and engineering high temperature Kondo many-body states.

cond-mat.str-el↗

arXiv2026

Strongly-coupled hybrid lattice-plasmons in layered cuprates

Metallic systems with delocalized valence electrons host collective charge density oscillations known as plasmons. On the other hand, conventional insulators do not have free electrons and the low energy charge degrees of freedom are pinned to the ions. The fate of the collective charge excitations in the intermediate regime is an outstanding question. This problem is especially important for strongly correlated systems such as the layered cuprates, where unconventional superconductivity and other emergent phenomena arise from valence electrons on the border between Mott localization and itinerancy. Using resonant inelastic X-ray scattering, we track this evolution in the prototypical electron-doped cuprate Nd2-xCexCuO4. We find a continuous transformation of the low-energy charge response: from an acoustic plasmon in the metallic regime, to a gapped hybrid mode at intermediate doping, and finally to a nearly dispersionless 139 meV excitation at half filling. Remarkably, the 139 meV excitation has approximately twice the energy of the oxygen breathing phonon responsible for the dispersion kink observed in angle-resolved photoemission spectroscopy, and is consistent with a putative 2-phonon excitation observed in Raman spectroscopy. These results establish a unified picture of collective charge excitations across the phase diagram of electron-doped cuprates, showing that such modes persist across the Mott transition via strong coupling to lattice degrees of freedom and revealing a missing link in the charge dynamics of carrier doped Mott insulators.

cond-mat.str-el↗

arXiv2024

Contrasting electron-phonon interaction between electron- and hole-doped cuprates

Spin- and charge-lattice interactions are potential key factors in the microscopic mechanism of high-temperature superconductivity in cuprates. Although both interactions can dramatically shape the low-energy electronic structure, their phenomenological roles in superconductivity are usually investigated independently. Employing angle-resolved photoemission spectroscopy, we reveal the spectroscopic fingerprint of short-range antiferromagnetic order in conjunction with enhanced electron-phonon interaction in the electron-doped cuprate superconductor $\mathrm{Nd_{1.85}Ce_{0.15}CuO_4}$. The observed mode coupling exhibits a strong momentum dependence that is in striking contrast to the node-antinode dichotomy previously observed in the hole-doped cuprates. Our results reveal an intimate relationship between electron-phonon coupling and antiferromagnetic fluctuations, which collectively sets the stage for unconventional superconductivity in the electron-doped cuprates.

cond-mat.supr-con↗

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

Electrical transport signatures of metallic surface state formation in the strongly-correlated insulator FeSb2

We present local and nonlocal electrical transport measurements of the correlated insulator FeSb$_2$. By employing wiring configurations that delineate between bulk- and surface-dominated conduction, we reveal the formation of a metallic surface state in FeSb$_2$ for temperatures $\lessapprox 5$~K. This result is corroborated by an angular rotation study of this material's magnetotransport, which also shows signatures of the transition from bulk- to surface-dominated conduction over the same temperature interval as the local/nonlocal transport divergence. Notable similarities with the topological Kondo insulator candidate SmB$_6$ are discussed.

cond-mat.str-el↗

arXiv2023

Anomalous normal state gap in an electron-doped cuprate

In the underdoped n-type cuprate Nd2-xCexCuO4, long-ranged antiferromagnetic order reconstructs the Fermi surface, resulting in a putative antiferromagnetic metal with small pockets. Using angle-resolved photoemission spectroscopy, we observe an anomalous energy gap, an order of magnitude smaller than the antiferromagnetic gap, in a wide range of the underdoped regime and smoothly connecting to the superconducting gap at optimal doping. After carefully considering all the known ordering tendencies in tandem with the phase diagram, we hypothesize that the normal state gap in the underdoped n-type cuprates originates from Cooper pairing. The high temperature scale of the normal state gap raises the prospect of engineering higher transition temperatures in the n-type cuprates comparable to that of the p-type cuprates.

cond-mat.supr-con↗

arXiv2023

Bogoliubov Quasiparticle on the Gossamer Fermi Surface in Electron-Doped Cuprates

In contrast to hole-doped cuprates, electron-doped cuprates consistently exhibit strong antiferromagnetic correlations with a commensurate (π, π) ordering wave vector, leading to the prevalent belief that antiferromagnetic spin fluctuations mediate Cooper pairing in these unconventional superconductors. However, early investigations produced two paradoxical findings: while antiferromagnetic spin fluctuations create the largest pseudogap at "hot spots" in momentum space, Raman scattering and angle-resolved photoemission spectroscopy measurements using the leading-edge method seem to suggest the superconducting gap is also maximized at these locations. This presented a dilemma for spin-fluctuation-mediated pairing: Cooper pairing is strongest at momenta where normal state low energy spectral weight is most suppressed. Here we investigate this dilemma in Nd2-xCexCuO4 using angle-resolved photoemission spectroscopy under significantly improved experimental conditions. The unprecedented signal-to-noise ratio and resolution allow us to directly observe the Bogoliubov quasiparticles, demonstrating the existence and importance of two sectors of states: 1. The reconstructed main band and the states gapped by the antiferromagnetic pseudogap around the hot spots. 2. The gossamer Fermi surface states with distinct dispersion inside the pseudogap, from which Bogoliubov quasiparticle coherence peaks emerge below Tc. Supported by numerical results, we propose that the non-zero modulus of the antiferromagnetic order parameter causes the former, while fluctuations in the antiferromagnetic order parameter orientation are responsible for the latter. Our revelations of the gossamer Fermi surface reconcile the paradoxical observations, deepening our understanding of superconductivity in electron-doped cuprates in particular, and unconventional superconductivity in general.

cond-mat.supr-con↗

arXiv2023

Differentiated roles of Lifshitz transition on thermodynamics and superconductivity in La2-xSrxCuO4

The effect of Lifshitz transition on thermodynamics and superconductivity in hole-doped cuprates has been heavily debated but remains an open question. In particular, an observed peak of electronic specific heat is proposed to originate from fluctuations of a putative quantum critical point p* (e.g. the termination of pseudogap at zero temperature), which is close to, but distinguishable from the Lifshitz transition in La-based cuprates. Here, we report an in situ angle-resolved photoemission spectroscopy study of three-dimensional Fermi surfaces in La2-xSrxCuO4 thin films(x = 0.06 - 0.35). With accurate kz dispersion quantification, the Lifshitz transition is determined to happen within a finite range around x = 0.21. Normal state electronic specific heat, calculated from spectroscopy-derived band parameters, agrees with previous thermodynamic microcalorimetry measurements. The account of the specific heat maximum by underlying band structures excludes the need for additionally dominant contribution from the quantum fluctuations at p*. A d-wave superconducting gap smoothly across the Lifshitz transition demonstrates the insensitivity of superconductivity to the dramatic density of states enhancement.

cond-mat.supr-con↗

arXiv2022

Thermal Hall conductivity of electron-doped cuprates

Measurements of the thermal Hall conductivity in hole-doped cuprates have shown that phonons acquire chirality in a magnetic field, both in the pseudogap phase and in the Mott insulator state. The microscopic mechanism at play is still unclear. A number of theoretical proposals are being considered, including skew scattering of phonons by various defects, the coupling of phonons to spins, and a state of loop-current order with the appropriate symmetries, but more experimental information is required to constrain theoretical scenarios. Here we present our study of the thermal Hall conductivity $κ_{\rm {xy}}$ in the electron-doped cuprates Nd$_{2-x}$Ce$_x$CuO$_4$ and Pr$_{2-x}$Ce$_x$CuO$_4$, for dopings across the phase diagram, from $x$ = 0, in the insulating antiferromagnetic phase, up to $x$ = 0.17, in the metallic phase above optimal doping. We observe a large negative thermal Hall conductivity at all dopings, in both materials. Since heat conduction perpendicular to the CuO$_2$ planes is dominated by phonons, the large thermal Hall conductivity we observe in electron-doped cuprates for a heat current in that direction must also be due to phonons, as in hole-doped cuprates. Measurements with a heat current perpendicular to the CuO$_2$ planes confirm that phonons are responsible for this thermal Hall signal, as in hole-doped cuprates. However, the degree of chirality, measured as the ratio $|κ_{\rm {xy}}$ / $κ_{\rm {xx}} |$, where $κ_{\rm {xx}}$ is the longitudinal thermal conductivity, is much larger in the electron-doped cuprates. We discuss various factors that may be involved in the mechanism that confers chirality to phonons in cuprates, including short-range spin correlations.

cond-mat.supr-con↗

arXiv2021

Intrinsic one-dimensional conducting channels in the Kondo insulator SmB6

Since its discovery as a Kondo insulator 50 years ago, SmB6 recently received a revival of interest due to detection of unexpected quantum oscillations in the insulating state, discovery of disorder-immune bulk transport, and proposals of correlation-driven topological physics. While recent transport results attribute the anomalous low temperature conduction to two-dimensional surface states, important alternatives, such as conduction channel residing in one-dimensional dislocation lines, have not been adequately explored. Here we study SmB6 with scanning microwave impedance microscopy and uncover evidence for conducting one-dimensional states terminating at surface step edges. These states remain conducting up to room temperature, indicating unusual robustness against scattering and an unconventional origin. Our results bring to light a heretofore undetected conduction route in SmB6 that contributes to the low temperature transport. The unique scenario of intrinsic one-dimensional conducting channels in a highly insulating correlated bulk offers a one-dimensional platform that may host exotic physics.

cond-mat.str-el↗

arXiv2020

Tuning time and energy resolution in time-resolved photoemission spectroscopy with nonlinear crystals

Time- and angle-resolved photoemission spectroscopy is a powerful probe of electronic band structures out of equilibrium. Tuning time and energy resolution to suit a particular scientific question has become an increasingly important experimental consideration. Many instruments use cascaded frequency doubling in nonlinear crystals to generate the required ultraviolet probe pulses. We demonstrate how calculations clarify the relationship between laser bandwidth and nonlinear crystal thickness contributing to experimental resolutions and place intrinsic limits on the achievable time-bandwidth product. Experimentally, we tune time and energy resolution by varying the thickness of nonlinear $β$-BaB$_2$O$_4$ crystals for frequency up-conversion, providing for a flexible experiment design. We achieve time resolutions of 58 to 103 fs and corresponding energy resolutions of 55 to 27 meV.

cond-mat.mtrl-sci↗

arXiv2020

Metallic surface states in a correlated d-electron topological Kondo insulator candidate FeSb2

The resistance of a conventional insulator diverges as temperature approaches zero. The peculiar low temperature resistivity saturation in the 4f Kondo insulator (KI) SmB6 has spurred proposals of a correlation-driven topological Kondo insulator (TKI) with exotic ground states. However, the scarcity of model TKI material families leaves difficulties in disentangling key ingredients from irrelevant details. Here we use angle-resolved photoemission spectroscopy (ARPES) to study FeSb2, a correlated d-electron KI candidate that also exhibits a low temperature resistivity saturation. On the (010) surface, we find a rich assemblage of metallic states with two-dimensional dispersion. Measurements of the bulk band structure reveal band renormalization, a large temperature-dependent band shift, and flat spectral features along certain high symmetry directions, providing spectroscopic evidence for strong correlations. Our observations suggest that exotic insulating states resembling those in SmB6 and YbB12 may also exist in systems with d instead of f electrons.

cond-mat.str-el↗