arXiv subjects

W. S. Lee

Publications and source records attributed to W. S. Lee.

At least 19 recordsLinked to original sources

arXiv2023

Universal orbital and magnetic structures in infinite-layer nickelates

We conducted a comparative study of the rare-earth infinite-layer nickelates films, RNiO2 (R = La, Pr, and Nd) using resonant inelastic X-ray scattering (RIXS). We found that the gross features of the orbital configurations are essentially the same, with minor variations in the detailed hybridization. For low-energy excitations, we unambiguously confirm the presence of damped magnetic excitations in all three compounds. By fitting to a linear spin-wave theory, comparable spin exchange coupling strengths and damping coefficients are extracted, indicating a universal magnetic structure in the infinite-layer nickelates. Interestingly, while signatures of a charge order are observed in LaNiO2 in the quasi-elastic region of the RIXS spectrum, it is absent in NdNiO2 and PrNiO2. This prompts further investigation into the universality and the origins of charge order within the infinite-layer inickelates.

cond-mat.str-el↗

arXiv2021

Soft X-ray Spectroscopy of Low-Valence Nickelates

Low-valence nickelates $-$ including infinite-layer (IL) and trilayer (TL) compounds $-$ are longstanding candidates for mimicking the high-temperature superconductivity of cuprates. A recent breakthrough in the field came with the discovery of superconductivity in hole-doped IL nickelates. Yet, the degree of similarity between low-valence nickelates and cuprates is the subject of a profound debate for which soft x-ray spectroscopy experiments at the Ni $L$- and O $K$-edge provided critical input. In this review, we will discuss the essential elements of the electronic structure of low-valance nickelates revealed by x-ray absorption spectroscopy (XAS) and resonant inelastic x-ray scattering (RIXS). Furthermore, we will review magnetic excitations observed in the RIXS spectra of IL and TL nickelates, which exhibit characteristics that are partly reminiscent of those of cuprates.

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arXiv2021

Magnetic excitations in infinite-layer nickelates

The discovery of superconductivity in infinite-layer nickelates brings us tantalizingly close to a new material class that mirrors the cuprate superconductors. Here, we report on magnetic excitations in these nickelates, measured using resonant inelastic x-ray scattering (RIXS) at the Ni L3-edge, to shed light on the material complexity and microscopic physics. Undoped NdNiO2 possesses a branch of dispersive excitations with a bandwidth of approximately 200 meV, reminiscent of strongly-coupled, antiferromagnetically aligned spins on a square lattice, despite a lack of evidence for long range magnetic order. The significant damping of these modes indicates the importance of coupling to rare-earth itinerant electrons. Upon doping, the spectral weight and energy decrease slightly, while the modes become overdamped. Our results highlight the role of Mottness in infinite-layer nickelates.

cond-mat.supr-con↗

arXiv2020

Orbital and Spin Character of Doped Carriers in Infinite-Layer Nickelates

The recent discovery of superconductivity in Nd$_{1-x}$Sr$_{x}$NiO$_2$ has drawn significant attention in the field. A key open question regards the evolution of the electronic structure with respect to hole doping. Here, we exploit x-ray absorption spectroscopy (XAS) and resonant inelastic x-ray scattering (RIXS) to probe the doping dependent electronic structure of the NiO$_2$ planes. Upon doping, a higher energy feature in Ni $L_3$ edge XAS develops in addition to the main absorption peak. By comparing our data to atomic multiplet calculations including $D_{4h}$ crystal field, the doping induced feature is consistent with a $d^8$ spin singlet state, in which doped holes reside in the $d_{x^2-y^2}$ orbitals, similar to doped single band Hubbard models. This is further supported by orbital excitations observed in RIXS spectra, which soften upon doping, corroborating with Fermi level shift associated with increasing holes in the $d_{x^2-y^2}$ orbital.

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arXiv2020

Spectroscopic Evidence for Charge Order Melting via Quantum Fluctuations in a Cuprate

Copper-oxide high TC superconductors possess a number of exotic orders co-existing with or proximal to superconductivity, whose quantum fluctuations may account for the unusual behaviors of the normal state, even affecting superconductivity. Yet, spectroscopic evidence about such quantum fluctuations remains elusive. Here, we reveal spectroscopic fingerprints for such fluctuations associated with a charge order (CO) in nearly optimally-doped Bi2Sr2CaCu2O8+d, using resonant inelastic x-ray scattering (RIXS). In the superconducting state, while the quasi-elastic CO signal decreases with temperature, the interplay between CO fluctuations and bond-stretching phonons in the form of a Fano-like interference paradoxically increases, incompatible with expectations for competing orders. Invoking general principles, we argue that this behavior reflects the properties of a dissipative system near an order-disorder quantum critical point, where the dissipation varies with the opening of the pseudogap and superconducting gap at low temperatures, leading to the proliferation of quantum critical fluctuations which melt CO.

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arXiv2019

Electronic structure of the parent compound of superconducting infinite-layer nickelates

The search for oxide materials with physical properties similar to the cuprate high Tc superconductors, but based on alternative transition metals such as nickel, has grown and evolved over time. The recent discovery of superconductivity in doped infinite-layer nickelates RNiO2 (R = rare-earth element) further strengthens these efforts.With a crystal structure similar to the infinite-layer cuprates - transition metal oxide layers separated by a rare-earth spacer layer - formal valence counting suggests that these materials have monovalent Ni1+ cations with the same 3d electron count as Cu2+ in the cuprates. Here, we use x-ray spectroscopy in concert with density functional theory to show that the electronic structure of RNiO2 (R = La, Nd), while similar to the cuprates, includes significant distinctions. Unlike cuprates with insulating spacer layers between the CuO2 planes, the rare-earth spacer layer in the infinite-layer nickelate supports a weakly-interacting three-dimensional 5d metallic state. This three-dimensional metallic state hybridizes with a quasi-two-dimensional, strongly correlated state with 3dx2-y2 symmetry in the NiO2 layers. Thus, the infinite-layer nickelate can be regarded as a sibling of the rare earth intermetallics, well-known for heavy Fermion behavior, where the NiO2 correlated layers play an analogous role to the 4f states in rare-earth heavy Fermion compounds. This unique Kondo- or Anderson-lattice-like "oxide-intermetallic" replaces the Mott insulator as the reference state from which superconductivity emerges upon doping.

cond-mat.supr-con↗

arXiv2018

Three dimensional collective charge excitations in electron-doped cuprate superconductors

High temperature cuprate superconductors consist of stacked CuO2 planes, with primarily two dimensional electronic band structures and magnetic excitations, while superconducting coherence is three dimensional. This dichotomy highlights the importance of out-of-plane charge dynamics, believed to be incoherent in the normal state, yet lacking a comprehensive characterization in energy-momentum space. Here, we use resonant inelastic x-ray scattering (RIXS) with polarization analysis to uncover the pure charge character of a recently discovered collective mode in electron-doped cuprates. This mode disperses along both the in- and, importantly, out-of-plane directions, revealing its three dimensional nature. The periodicity of the out-of-plane dispersion corresponds to the CuO2 plane distance rather than the crystallographic c-axis lattice constant, suggesting that the interplane Coulomb interaction drives the coherent out-of-plane charge dynamics. The observed properties are hallmarks of the long-sought acoustic plasmon, predicted for layered systems and argued to play a substantial role in mediating high temperature superconductivity.

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arXiv2016

Arithmetic completely regular codes

In this paper, we explore completely regular codes in the Hamming graphs and related graphs. Experimental evidence suggests that many completely regular codes have the property that the eigenvalues of the code are in arithmetic progression. In order to better understand these "arithmetic completely regular codes", we focus on cartesian products of completely regular codes and products of their corresponding coset graphs in the additive case. Employing earlier results, we are then able to prove a theorem which nearly classifies these codes in the case where the graph admits a completely regular partition into such codes (e.g, the cosets of some additive completely regular code). Connections to the theory of distance-regular graphs are explored and several open questions are posed.

math.CO↗

arXiv2015

Raman and fluorescence characteristics of resonant inelastic X-ray scattering from doped superconducting cuprates

Measurements of spin excitations are essential for an understanding of spin-mediated pairing for superconductivity; and resonant inelastic X-ray scattering (RIXS) provides a considerable opportunity to probe high-energy spin excitations. However, whether RIXS correctly measures the collective spin excitations of doped superconducting cuprates remains under debate. Here we demonstrate distinct Raman- and fluorescence-like RIXS excitations of Bi$_{1.5}$Pb$_{0.6}$Sr$_{1.54}$CaCu$_{2}$O$_{8+δ}$ in the mid-infrared energy region. Combining photon-energy and momentum dependent RIXS measurements with theoretical calculations using exact diagonalization provides conclusive evidence that the Raman-like RIXS excitations correspond to collective spin excitations, which are magnons in the undoped Mott insulators and evolve into paramagnons in doped superconducting compounds. In contrast, the fluorescence-like shifts are due primarily to the continuum of particle-hole excitations in the charge channel. Our results show that under the proper experimental conditions RIXS indeed can be used to probe paramagnons in doped high-$T_c$ cuprate superconductors.

cond-mat.supr-con↗

arXiv2015

Spatially resolved ultrafast magnetic dynamics launched at a complex-oxide hetero-interface

Static strain in complex oxide heterostructures has been extensively used to engineer electronic and magnetic properties at equilibrium. In the same spirit, deformations of the crystal lattice with light may be used to achieve functional control across hetero-interfaces dynamically. Here, by exciting large amplitude infrared-active vibrations in a LaAlO3 substrate we induce magnetic order melting in a NdNiO3 film across a hetero-interface. Femtosecond Resonant Soft X-ray Diffraction is used to determine the spatial and temporal evolution of the magnetic disordering. We observe a magnetic melt front that grows from the substrate interface into the film, at a speed that suggests electronically driven propagation. Light control and ultrafast phase front propagation at hetero-interfaces may lead to new opportunities in optomagnetism, for example by driving domain wall motion to transport information across suitably designed devices.

cond-mat.str-el↗

arXiv2015

Melting of Charge Stripes in Vibrationally Driven La1.875Ba0.125CuO4: Assessing the Respective Roles of Electronic and Lattice Order in Frustrated Superconductors

We report femtosecond resonant soft X-ray diffraction measurements of the dynamics of the charge order and of the crystal lattice in non-superconducting, stripe-ordered La1.875Ba0.125CuO4. Excitation of the in-plane Cu-O stretching phonon with a mid-infrared pulse has been previously shown to induce a transient superconducting state in the closely related compound La1.675Eu0.2Sr0.125CuO4. In La1.875Ba0.125CuO4, we find that the charge stripe order melts promptly on a sub-picosecond time scale. Surprisingly, the low temperature tetragonal distortion is only weakly reduced, reacting on significantly longer time scales that do not correlate with light-induced superconductivity. This experiment suggests that charge modulations alone, and not the LTT distortion, prevent superconductivity in equilibrium.

cond-mat.supr-con↗

arXiv2014

Asymmetry of collective excitations in electron and hole doped cuprate superconductors

High-temperature superconductivity (HTSC) mysteriously emerges upon doping holes or electrons into insulating copper oxides with antiferromagnetic (AFM) order. It has been thought that the large energy scale of magnetic excitations, compared to phonon energies for example, lies at the heart of an electronically-driven superconducting phase at high temperatures. However, despite extensive studies, little information is available for comparison of high-energy magnetic excitations of hole- and electron-doped superconductors to assess a possible correlation with the respective superconducting transition temperatures. Here, we use resonant inelastic x-ray scattering (RIXS) at the Cu L3-edge to reveal high-energy collective excitations in the archetype electron-doped cuprate Nd2-xCexCuO4 (NCCO). Surprisingly, despite the fact that the spin stiffness is zero and the AFM correlations are short-ranged, magnetic excitations harden significantly across the AFM-HTSC phase boundary, in stark contrast with the hole-doped cuprates. Furthermore, we find an unexpected and highly dispersive mode in superconducting NCCO that is undetected in the hole-doped compounds, which emanates from the zone center with a characteristic energy comparable to the pseudogap, and may signal a quantum phase distinct from superconductivity. The uncovered asymmetry in the high-energy collective excitations with respect to hole and electron doping provides additional constraints for modeling the HTSC cuprates.

cond-mat.supr-con↗

arXiv2014

Angle-resolved photoemission spectroscopy study of HgBa$_{2}$CuO$_{4+δ}$

HgBa$_{2}$CuO$_{4+δ}$ (Hg1201) has been shown to be a model cuprate for scattering, optical, and transport experiments, but angle-resolved photoemission spectroscopy (ARPES) data are still lacking owing to the absence of a charge-neutral cleavage plane. We report on progress in achieving the experimental conditions for which quasiparticles can be observed in the near-nodal region of the Fermi surface. The d-wave superconducting gap is measured and found to have a maximum of 39 meV. At low temperature, a kink is detected in the nodal dispersion at approximately 51 meV below the Fermi level, an energy that is different from other cuprates with comparable T$_c$. The superconducting gap, Fermi surface, and nodal band renormalization measured here provide a crucial momentum-space complement to other experimental probes.

cond-mat.supr-con↗

arXiv2013

Charge-orbital-lattice coupling effects in the dd-excitation profile of one dimensional cuprates

We identify dd-excitations in the quasi-one dimensional compound Ca$_2$Y$_2$Cu$_5$O$_{10}$ using resonant inelastic x-ray scattering. By tuning across the Cu L$_3$-edge, we observe abrupt shifts in the dd-peak positions as a function of incident photon energy. This observation demonstrates orbital-specific coupling of the high-energy excited states of the system to the low-energy degrees of freedom. A Franck-Condon treatment of electron-lattice coupling, consistent with other measurements in this compound, reproduces these shifts, explains the Gaussian lineshapes, and highlights charge-orbital-lattice renormalization in the high energy d-manifold.

cond-mat.str-el↗

arXiv2013

Real-time manifestation of strongly coupled spin and charge order parameters in stripe-ordered nickelates via time-resolved resonant x-ray diffraction

We investigate the order parameter dynamics of the stripe-ordered nickelate, La$_{1.75}$Sr$_{0.25}$NiO$_4$, using time-resolved resonant X-ray diffraction. In spite of distinct spin and charge energy scales, the two order parameters' amplitude dynamics are found to be linked together due to strong coupling. Additionally, the vector nature of the spin sector introduces a longer re-orientation time scale which is absent in the charge sector. These findings demonstrate that the correlation linking the symmetry-broken states does not unbind during the non-equilibrium process, and the time scales are not necessarily associated with the characteristic energy scales of individual degrees of freedom.

cond-mat.str-el↗

arXiv2013

The Role of Lattice Coupling in Establishing Electronic and Magnetic Properties in Quasi-One-Dimensional Cuprates

High resolution resonant inelastic x-ray scattering has been performed to reveal the role of lattice-coupling in a family of quasi-1D insulating cuprates, Ca$_{2+5x}$Y$_{2-5x}$Cu$_5$O$_{10}$. Site-dependent low energy excitations arising from progressive emissions of a 70 meV lattice vibrational mode are resolved for the first time, providing a direct measurement of electron-lattice coupling strength. We show that such electron-lattice coupling causes doping-dependent distortions of the Cu-O-Cu bond angle, which sets the intra-chain spin exchange interactions. Our results indicate that the lattice degrees of freedom are fully integrated into the electronic behavior in low dimensional systems.

cond-mat.str-el↗

arXiv2012

Phase competition in trisected superconducting dome

A detailed phenomenology of low energy excitations is a crucial starting point for microscopic understanding of complex materials such as the cuprate high temperature superconductors. Because of its unique momentum-space discrimination, angle-resolved photoemission spectroscopy (ARPES) is ideally suited for this task in the cuprates where emergent phases, particularly superconductivity and the pseudogap, have anisotropic gap structure in momentum space. We present a comprehensive doping-and-temperature dependence ARPES study of spectral gaps in Bi$_2$Sr$_2$CaCu$_2$O$_{8+δ}$ (Bi-2212), covering much of the superconducting portion of the phase diagram. In the ground state, abrupt changes in near-nodal gap phenomenology give spectroscopic evidence for two potential quantum critical points, p$=$0.19 for the pseudogap phase and p$=$0.076 for another competing phase. Temperature dependence reveals that the pseudogap is not static below T$_c$ and exists p$>$0.19 at higher temperatures. Our data imply a revised phase diagram which reconciles conflicting reports about the endpoint of the pseudogap in the literature, incorporates phase competition between the superconducting gap and pseudogap, and highlights distinct physics at the edge of the superconducting dome.

cond-mat.supr-con↗

arXiv2012

Phase Fluctuations and the Absence of Topological Defects in Photo-excited Charge Ordered Nickelate

The dynamics of an order parameter's amplitude and phase determines the collective behaviour of novel states emerged in complex materials. Time- and momentum-resolved pump-probe spectroscopy, by virtue of its ability to measure material properties at atomic and electronic time scales and create excited states not accessible by the conventional means can decouple entangled degrees of freedom by visualizing their corresponding dynamics in the time domain. Here, combining time-resolved femotosecond optical and resonant x-ray diffraction measurements on striped La1.75Sr0.25NiO4, we reveal unforeseen photo-induced phase fluctuations of the charge order parameter. Such fluctuations preserve long-range order without creating topological defects, unlike thermal phase fluctuations near the critical temperature in equilibrium10. Importantly, relaxation of the phase fluctuations are found to be an order of magnitude slower than that of the order parameter's amplitude fluctuations, and thus limit charge order recovery. This discovery of new aspect to phase fluctuation provides more holistic view for the importance of phase in ordering phenomena of quantum matter.

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