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Orbital-specific Itinerancy and Localization in a Kagome Magnet
Authors:
S. V. Streltsov,
H. Y. Huang,
A. Ushakov,
C. I. Wu,
A. Singh,
J. Su,
J. Okamoto,
C. T. Chen,
K. Wang,
A. I. Poteryaev,
S-W. Cheong,
A. Fujimori,
D. J. Huang
Abstract:
The kagome lattice naturally hosts flat bands, Dirac fermions, and van Hove singularities, yet whether its geometry can stabilize orbital-selective phases - a hallmark of Hund's physics in multi-orbital correlated systems - has remained an open question. Here, we combine resonant inelastic X-ray scattering with density functional theory and dynamical mean-field theory to demonstrate that YMn$_6$Sn…
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The kagome lattice naturally hosts flat bands, Dirac fermions, and van Hove singularities, yet whether its geometry can stabilize orbital-selective phases - a hallmark of Hund's physics in multi-orbital correlated systems - has remained an open question. Here, we combine resonant inelastic X-ray scattering with density functional theory and dynamical mean-field theory to demonstrate that YMn$_6$Sn$_6$ exhibits a spontaneous orbital differentiation into coexisting itinerant and localized electrons within the same Mn $3d$ manifold. Orbitals directed along Mn-Mn bonds provide coherent quasiparticles and metallic bands, while those pointing toward ligands become strongly correlated and display non-Fermi-liquid behavior. Hund's intra-atomic exchange suppresses orbital fluctuations, stabilizing this dichotomy and providing a natural double-exchange-like mechanism for the observed ferromagnetic bilayer coupling. Our work establishes YMn$_6$Sn$_6$ as a kagome platform where orbital selectivity, flat-band topology, and Hund's metallicity converge - revealing that geometric frustration and correlation-driven orbital differentiation can cooperatively design exotic quantum phases beyond the canonical paradigms of Mott physics or band topology alone.
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Submitted 22 March, 2026;
originally announced March 2026.
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Quantum critical behavior of cuprate superconductors observed by inelastic X-ray scattering
Authors:
H. Y. Huang,
C. Y. Mou,
A. Singh,
J. S. Su,
J. Okamoto,
S. Komiya,
C. T. Chen,
T. K. Lee,
A. Fujimori,
D. J. Huang
Abstract:
Progress toward a complete understanding of cuprate superconductors has been hindered by their intricate phase diagram, potentially linked to a quantum critical point (QCP). However, conclusive evidence for the QCP is lacking, as the presumed QCP is buried under the superconducting dome, disguising its presence. Here, we use high-resolution resonant inelastic X-ray scattering to examine the dynami…
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Progress toward a complete understanding of cuprate superconductors has been hindered by their intricate phase diagram, potentially linked to a quantum critical point (QCP). However, conclusive evidence for the QCP is lacking, as the presumed QCP is buried under the superconducting dome, disguising its presence. Here, we use high-resolution resonant inelastic X-ray scattering to examine the dynamical charge-charge correlation in La$_{2-x}$Sr$_x$CuO$_4$ and uncover the quantum critical scaling, a key feature required for a QCP. Specifically, \djh{we observed that the inverse correlation lengths for various dopings and temperatures collapsed onto a universal scaling curve, yielding a critical exponent $ν$ of $0.74 \pm 0.08$. The non-negativity of this exponent confirms the presence of a QCP. Remarkably, the value of $ν$ suggests that while the QCP is manifested through the charge-density wave, other orders also participate, such that the QCP appears to belong to the universality class characterized by the O(4) symmetry, reminiscent of the microscopic SO(4) symmetry in the Hubbard model at half-filling. Further analysis indicates that the QCP is highly dissipative with a short quasi-particle lifetime, reflecting the intertwined quantum fluctuations due to its being buried inside the superconducting state.
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Submitted 25 February, 2026; v1 submitted 11 February, 2026;
originally announced February 2026.
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Non-reciprocal circular dichroism of axial phonons coupled to ferro-rotational order
Authors:
H. Y. Huang,
G. Channagowdra,
D. Banerjee,
E. V. Komleva,
J. Okamoto,
C. T. Chen,
M. Guennou,
S. Johnston,
S. V. Streltsov,
C. Y. Mou,
A. Fujimori,
S-W. Cheong,
D. J. Huang
Abstract:
Circular dichroism (CD) in X-ray absorption, defined as the difference in absorption between opposite circular polarizations, is fundamentally enabled by the breaking of time-reversal symmetry or inversion symmetry. It is therefore sensitive to magnetism, chirality, and their interplay. In contrast, the sample symmetry alone is insufficient to determine whether CD in resonant inelastic X-ray scatt…
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Circular dichroism (CD) in X-ray absorption, defined as the difference in absorption between opposite circular polarizations, is fundamentally enabled by the breaking of time-reversal symmetry or inversion symmetry. It is therefore sensitive to magnetism, chirality, and their interplay. In contrast, the sample symmetry alone is insufficient to determine whether CD in resonant inelastic X-ray scattering (RIXS) is allowed. Rather, RIXS-CD is governed by both the sample symmetry and the scattering geometry. Here, using RIXS, we identify circularly polarized phonons coupled to ferro-rotational order in MnTiO$_3$, which we refer to as ferro-axial phonons. Their excitations provide a direct demonstration of non-reciprocal RIXS-CD, in which the dichroic response changes upon reversing the propagation direction of the incident X-rays, although the system globally preserves both inversion and time-reversal symmetries. We propose that a condensate of these phonons, manifested as standing waves, underlies the ferro-rotational order in MnTiO$_3$. The observed non-reciprocal CD reflects the interplay among photon helicity, phonon polarization, and ferro-rotational order.
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Submitted 7 August, 2026; v1 submitted 26 December, 2025;
originally announced December 2025.
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Bi-altermagnetism unveiled by sublattice-specific circular dichroism in resonant inelastic X-ray scattering
Authors:
G. Channagowdra,
A. Singh,
H. Y. Huang,
M. Furo,
Bin Gao,
Pengcheng Dai,
C. T. Chen,
J. Kunes,
A. Fujimori,
S-W. Cheong,
A. Hariki,
D. J. Huang
Abstract:
An altermagnet is a recently identified class of magnets that exhibit a zero net magnetic moment but break symmetry under the combined operations of parity and time reversal. It typically consists of two magnetic sites of opposite spins related by rotation within the unit cell. Here, we use circular dichroism (CD) in resonant inelastic X-ray scattering (RIXS) to identify a new form of altermagneti…
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An altermagnet is a recently identified class of magnets that exhibit a zero net magnetic moment but break symmetry under the combined operations of parity and time reversal. It typically consists of two magnetic sites of opposite spins related by rotation within the unit cell. Here, we use circular dichroism (CD) in resonant inelastic X-ray scattering (RIXS) to identify a new form of altermagnetism, namely bi-altermagnetism, in the correlated insulator Fe2Mo3O8, which comprises two altermagnetic sublattices: one with alternating quasi-octahedral Fe environments and the other with alternating tetrahedral Fe environments. We experimentally revealed the emergence of CD in an achiral, zero-magnetization system, thereby probing mirror-symmetry breaking associated with altermagnetic order. Notably, the CD appeared at sublattice-specific excitations of the octahedral and tetrahedral sites, indicating symmetry breaking in both altermagnetic sublattices. Calculations based on a model with the bi-altermagnetic order along the c axis successfully reproduce the observed CD. Our findings provide compelling evidence for bi-altermagnetism in Fe2Mo3O8, and showcase the use of RIXS-CD as a probe of magnetic sublattices in systems with zero net magnetization.
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Submitted 1 May, 2026; v1 submitted 30 November, 2025;
originally announced December 2025.
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Altermagnetic boosting of chiral phonons
Authors:
J. Okamoto,
C. Y. Mou,
H. Y. Huang,
G. Channagowdra,
C. Won,
K. Du,
X. Fang,
E. V. Komleva,
C. T. Chen,
S. V. Streltsov,
A. Fujimori,
S-W. Cheong,
D. J. Huang
Abstract:
Chirality characterizes the asymmetry between a structure and its mirror image and underlies a wide range of chiral functionalities. In crystallographically chiral materials, phonons with non-zero linear momentum $\textbf{k}$ can acquire a $k$-induced longitudinal magnetization, giving rise to chiral phonons. Helical spin order, with its proper screw-type configuration, breaks all mirror symmetrie…
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Chirality characterizes the asymmetry between a structure and its mirror image and underlies a wide range of chiral functionalities. In crystallographically chiral materials, phonons with non-zero linear momentum $\textbf{k}$ can acquire a $k$-induced longitudinal magnetization, giving rise to chiral phonons. Helical spin order, with its proper screw-type configuration, breaks all mirror symmetries and therefore carries magnetic chirality. Such helical spins also generate non-relativistic spin splitting for any quasiparticle excitations propagating along the screw axis. To explore the possible connection between chiral phonons and magnetic chirality, we investigated the crystallographically polar and chiral compound (Mn,Ni)$_3$TeO$_6$, which hosts three distinct states: a paramagnetic state, a helical spin state with magnetic chirality, and a collinear spin state without magnetic chirality. We find an approximately tenfold enhancement of chiral-phonon coupling in the helical spin state along the screw axis, compared with both the paramagnetic and collinear spin states. These results identify a new route to amplify chiral phonons through an altermagnetic effect arising from the broken parity-time symmetry in helical spins. %from non-relativistic spin splitting.
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Submitted 29 November, 2025;
originally announced December 2025.
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Bimagnon dispersion of La2CuO4 probed by resonant inelastic X-ray scattering
Authors:
A. Singh,
H. Y. Huang,
K. Tsutsui,
T. Tohyama,
S. Komiya,
J. Okamoto,
C. T. Chen,
A. Fujimori,
D. J. Huang
Abstract:
We report on the study of the magnetic excitations of Mott insulator La2CuO4 by using resonant inelastic x-ray scattering (RIXS) and cluster calculations within the framework of exact diagonalization. Our results demonstrate experimentally that the bimagnon excitation in Cu L-edge RIXS is enhanced if the incident x-ray energy is slightly above the absorption edge. Through incident-energy-dependent…
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We report on the study of the magnetic excitations of Mott insulator La2CuO4 by using resonant inelastic x-ray scattering (RIXS) and cluster calculations within the framework of exact diagonalization. Our results demonstrate experimentally that the bimagnon excitation in Cu L-edge RIXS is enhanced if the incident x-ray energy is slightly above the absorption edge. Through incident-energy-dependent momentum-resolved RIXS, we investigated the excitation of the bimagnon with predominantly A1 symmetry. The bimagnons of La2CuO4 exhibit a nearly flat dispersion with momentum along the Cu-O bond direction. This observation agrees with the bimagnon dispersion from the calculations on a single-band Hubbard model rather than a Heisenberg model with only the nearest neighbor exchange interaction. This means that the effect of the higher-order spin couplings such as the cyclic or ring exchange interactions caused by the coherent motion of electrons beyond nearest-neighbor sites is important for understanding the bimagnon dynamics of cuprates.
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Submitted 3 October, 2025;
originally announced October 2025.
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Out-of-phase Plasmon Excitations in the Trilayer Cuprate Bi$_2$Sr$_2$Ca$_2$Cu$_3$O$_{10+δ}$
Authors:
S. Nakata,
M. Bejas,
J. Okamoto,
K. Yamamoto,
D. Shiga,
R. Takahashi,
H. Y. Huang,
H. Kumigashira,
H. Wadati,
J. Miyawaki,
S. Ishida,
H. Eisaki,
A. Fujimori,
A. Greco,
H. Yamase,
D. J. Huang,
H. Suzuki
Abstract:
Within a homologous series of cuprate superconductors, variations in the stacking of CuO$_2$ layers influence the collective charge dynamics through the long-range Coulomb interactions. We use O $K$-edge resonant inelastic x-ray scattering to reveal plasmon excitations in the optimally-doped trilayer Bi$_2$Sr$_2$Ca$_2$Cu$_3$O$_{10+δ}$. The observed plasmon exhibits nearly $q_z$-independent dispers…
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Within a homologous series of cuprate superconductors, variations in the stacking of CuO$_2$ layers influence the collective charge dynamics through the long-range Coulomb interactions. We use O $K$-edge resonant inelastic x-ray scattering to reveal plasmon excitations in the optimally-doped trilayer Bi$_2$Sr$_2$Ca$_2$Cu$_3$O$_{10+δ}$. The observed plasmon exhibits nearly $q_z$-independent dispersion and a large excitation gap of approximately 300 meV. This mode is primarily ascribed to the $ω_{-}$ mode, where the charge density on the outer CuO$_2$ sheets oscillates out of phase while the density in the inner sheet remains unaltered at $q_z=0$. The intensity of the acoustic $ω_3$ mode is relatively weak and becomes vanishingly small near $(q_x, q_y)=(0, 0)$. This result highlights a qualitative change in the eigenmode of the dominant low-energy plasmon with the number of CuO$_2$ layers.
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Submitted 11 February, 2025; v1 submitted 5 February, 2025;
originally announced February 2025.
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Spin-orbit-entangled electronic structure of Ba$_2$CaOsO$_6$ studied by O $K$-edge resonant inelastic X-ray scattering
Authors:
J. Okamoto,
G. Shibata,
Yu. S. Posonov,
H. Hayashi,
K. Yamaura,
H. Y. Huang,
A. Singh,
C. T. Chen,
A. Tanaka,
S. V. Streltsov,
D. J. Huang,
A. Fujimori
Abstract:
Transition-metal ions with $5d^2$ electronic configuration in a cubic crystal field are prone to have a vanishing dipolar magnetic moment but finite higher-order multipolar moments, and they are expected to exhibit exotic physical properties. Through an investigation using resonant inelastic X-ray spectroscopy (RIXS), Raman spectroscopy, and theoretical ligand-field (LF) multiplet and $ab initio$…
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Transition-metal ions with $5d^2$ electronic configuration in a cubic crystal field are prone to have a vanishing dipolar magnetic moment but finite higher-order multipolar moments, and they are expected to exhibit exotic physical properties. Through an investigation using resonant inelastic X-ray spectroscopy (RIXS), Raman spectroscopy, and theoretical ligand-field (LF) multiplet and $ab initio$ calculations, we fully characterized the local electronic structure of Ba$_2$CaOsO$_6$, particularly, the crystal-field symmetry of the 5$d^2$ electrons in this anomalous material. The low-energy multiplet excitations from RIXS at the oxygen $K$ edge and Raman-active phonons both show no splitting. These findings are consistent with the ground state of Os ions dominated by magnetic octupoles. Obtained parameters pave the way for further realistic microscopic studies of this highly unusual class of materials, advancing our understanding of spin-orbit physics in systems with higher-order multipoles.
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Submitted 15 July, 2025; v1 submitted 17 December, 2024;
originally announced December 2024.
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Spin Excitations and Flat Electronic Bands in a Cr-based Kagome Superconductor
Authors:
Zehao Wang,
Yucheng Guo,
Hsiao Yu Huang,
Fang Xie,
Yuefei Huang,
Bin Gao,
Ji Seop Oh,
Han Wu,
Jun Okamoto,
Ganesha Channagowdra,
Chien Te Chen,
Feng Ye,
Xingye Lu,
Zhaoyu Liu,
Zheng Ren,
Yuan Fang,
Yiming Wang,
Ananya Biswas,
Yichen Zhang,
Ziqin Yue,
Cheng Hu,
Chris Jozwiak,
Aaron Bostwick,
Eli Rotenberg,
Makoto Hashimoto
, et al. (11 additional authors not shown)
Abstract:
In the quest for topology- and correlation-driven quantum states, kagome lattice materials have garnered significant interest for their band structures, featuring flat bands (FBs) from the quantum destructive interference of the electronic wavefunction. Tuning an FB to the chemical potential could induce electronic instabilities and emergent orders. Despite extensive studies, direct evidence of FB…
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In the quest for topology- and correlation-driven quantum states, kagome lattice materials have garnered significant interest for their band structures, featuring flat bands (FBs) from the quantum destructive interference of the electronic wavefunction. Tuning an FB to the chemical potential could induce electronic instabilities and emergent orders. Despite extensive studies, direct evidence of FBs tuned to the chemical potential and their role in emergent orders in bulk materials remains lacking. Using angle-resolved photoemission spectroscopy, resonant inelastic X-ray scattering, and density functional theory, we show that the low-energy structure of the Cr-based kagome metal superconductor {\Cr} is dominated by FBs at the Fermi level. We also observe low-energy magnetic excitations evolving across the low-temperature transition, largely consistent with the FB shift. Our results suggest that the low-temperature order contains a magnetic origin and that the kagome FBs may play a role in the emergence of this order.
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Submitted 24 November, 2025; v1 submitted 7 June, 2024;
originally announced June 2024.
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Exciton dynamics uncovering electron fractionalization in superconducting cuprates
Authors:
A. Singh,
H. Y. Huang,
J. D. Xie,
J. Okamoto,
C. T. Chen,
T. Watanabe,
A. Fujimori,
M. Imada,
D. J. Huang
Abstract:
Electron quasiparticles play a crucial role in simplifying the description of many-body physics in solids with surprising success. Conventional Landau's Fermi-liquid and quasiparticle theories for high-temperature superconducting cuprates have, however, received skepticism from various angles. A path-breaking framework of electron fractionalization has been established to replace the Fermi-liquid…
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Electron quasiparticles play a crucial role in simplifying the description of many-body physics in solids with surprising success. Conventional Landau's Fermi-liquid and quasiparticle theories for high-temperature superconducting cuprates have, however, received skepticism from various angles. A path-breaking framework of electron fractionalization has been established to replace the Fermi-liquid theory for systems that show the fractional quantum Hall effect and the Mott insulating phenomena; whether it captures the essential physics of the pseudogap and superconducting phases of cuprates is still an open issue. Here, we show that excitonic excitation of optimally doped Bi$_2$Sr$_2$CaCu$_2$O$_{8+δ}$ with energy far above the superconducting-gap energy scale, about 1 eV or even higher, is unusually enhanced by the onset of superconductivity. Our finding proves the involvement of such high-energy excitons in superconductivity. Therefore, the observed enhancement in the spectral weight of excitons imposes a crucial constraint on theories for the pseudogap and superconducting mechanisms. A simple two-component fermion model which embodies electron fractionalization in the pseudogap state well explains the change, pointing toward a novel route for understanding the electronic structure of superconducting cuprates.
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Submitted 26 July, 2022; v1 submitted 25 July, 2022;
originally announced July 2022.
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Quantum fluctuations of charge order induce phonon softening in a superconducting cuprate
Authors:
H. Y. Huang,
A. Singh,
C. Y. Mou,
S. Johnston,
A. F. Kemper,
J. van den Brink,
P. J. Chen,
T. K. Lee,
J. Okamoto,
Y. Y. Chu,
J. H. Li,
S. Komiya,
A. C. Komarek,
A. Fujimori,
C. T. Chen,
D. J. Huang
Abstract:
Quantum phase transitions play an important role in shaping the phase diagram of high-temperature cuprate superconductors. These cuprates possess intertwined orders which interact strongly with superconductivity. However, the evidence for the quantum critical point associated with the charge order in the superconducting phase remains elusive. Here we show the short-range charge orders and the spec…
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Quantum phase transitions play an important role in shaping the phase diagram of high-temperature cuprate superconductors. These cuprates possess intertwined orders which interact strongly with superconductivity. However, the evidence for the quantum critical point associated with the charge order in the superconducting phase remains elusive. Here we show the short-range charge orders and the spectral signature of the quantum fluctuations in La$_{2-x}$Sr$_x$CuO$_4$ (LSCO) near the optimal doping using high-resolution resonant inelastic X-ray scattering. On performing calculations through a diagrammatic framework, we discovered that the charge correlations significantly soften several branches of phonons. These results elucidate the role of charge order in the LSCO compound, providing evidence for quantum critical scaling and discommensurations associated with charge order.
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Submitted 26 September, 2021; v1 submitted 25 August, 2021;
originally announced August 2021.
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Acoustic plasmons and conducting carriers in hole-doped cuprate superconductors
Authors:
A. Singh,
H. Y. Huang,
Christopher Lane,
J. H. Li,
J. Okamoto,
S. Komiya,
Robert S. Markiewicz,
Arun Bansil,
A. Fujimori,
C. T. Chen,
D. J. Huang
Abstract:
The superconductivity of cuprates, which has been a mystery ever since its discovery decades ago, is created through doping electrons or holes into a Mott insulator. There, however, exists an inherent electron-hole asymmetry in cuprates. The layered crystal structures of cuprates enable collective charge excitations fundamentally different from those of three-dimensional metals, i.e., acoustic pla…
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The superconductivity of cuprates, which has been a mystery ever since its discovery decades ago, is created through doping electrons or holes into a Mott insulator. There, however, exists an inherent electron-hole asymmetry in cuprates. The layered crystal structures of cuprates enable collective charge excitations fundamentally different from those of three-dimensional metals, i.e., acoustic plasmons. Acoustic plasmons have been recently observed in electron-doped cuprates by resonant inelastic X-ray scattering (RIXS); in contrast, there is no evidence for acoustic plasmons in hole-doped cuprates, despite extensive measurements. This contrast led us to investigate whether the doped holes in cuprates La$_{2-x}$Sr$_x$CuO$_4$ are conducting carriers or are too incoherent to induce collective charge excitation. Here we present momentum-resolved RIXS measurements and calculations of collective charge response via the loss function to reconcile the aforementioned issues. Our results provide unprecedented spectroscopic evidence for the acoustic plasmons and long sought conducting p holes in hole-doped cuprates.
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Submitted 10 September, 2021; v1 submitted 23 June, 2020;
originally announced June 2020.
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Development of the Soft X-ray AGM-AGS RIXS Beamline at Taiwan Photon Source
Authors:
A. Singh,
H. Y. Huang,
Y. Y. Chu,
C. Y. Hua,
S. W. Lin,
H. S. Fung,
H. W. Shiu,
J. Chang,
J. H. Li,
J. Okamoto,
C. C. Chiu,
C. H. Chang,
W. B. Wu,
S. Y. Perng,
S. C. Chung,
K. Y. Kao,
S. C. Yeh,
H. Y. Chao,
J. H. Chen,
D. J. Huang,
C. T. Chen
Abstract:
We report on the development of a high-resolution and highly efficient beamline for soft-X-ray resonant inelastic X-ray scattering (RIXS) located at Taiwan Photon Source. This beamline adopts an optical design that uses an active grating monochromator (AGM) and an active grating spectrometer (AGS) to implement the energy compensation principle of grating dispersion. Active gratings are utilized to…
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We report on the development of a high-resolution and highly efficient beamline for soft-X-ray resonant inelastic X-ray scattering (RIXS) located at Taiwan Photon Source. This beamline adopts an optical design that uses an active grating monochromator (AGM) and an active grating spectrometer (AGS) to implement the energy compensation principle of grating dispersion. Active gratings are utilized to diminish defocus, coma and higher-order aberrations as well as to decrease the slope errors caused by thermal deformation and optical polishing. The AGS is mounted on a rotatable granite platform to enable momentum-resolved RIXS measurements with scattering angle over a wide range. Several high-precision instruments developed in house for this beamline are briefly described. The best energy resolution obtained from this AGM-AGS beamline was 12.4 meV at 530 eV, achieving a resolving power 42,000, while the bandwidth of the incident soft X-rays was kept at 0.5 eV. To demonstrate the scientific impacts of high-resolution RIXS, we present an example of momentum-resolved RIXS measurements on a high-temperature superconducting cuprate, La$_{2-x}$Sr$_x$CuO$_4$. The measurements reveal the A$_{1g}$ apical oxygen phonons in superconducting cuprates, opening a new opportunity to investigate the coupling between these phonons and charge density waves.
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Submitted 24 June, 2020; v1 submitted 23 June, 2020;
originally announced June 2020.
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Evolution of valence-specific spin states and local distortions in La$_{2-x}$Sr$_x$CoO$_4$
Authors:
J. Okamoto,
A. Chainani,
Z. Y. Chen,
H. Y. Huang,
A. Singh,
T. Sasagawa,
D. I. Khomskii,
A. Fujimori,
C. T. Chen,
D. J. Huang
Abstract:
We present X-ray spectroscopic evidence for the evolution of valence-specific spin states and tetragonal distortions in single-layer cobaltates. Measurements of Co $L_3$-edge resonant inelastic X-ray scattering reveal the $t_{2g}$ electronic structure of Co for hole-doped La$_{2-x}$Sr$_x$CoO$_4$ ($x$ = 0.5, 0.7 and 0.8). As the Sr-doping $x$ increases, the tetragonal splitting of the $t_{2g}$ stat…
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We present X-ray spectroscopic evidence for the evolution of valence-specific spin states and tetragonal distortions in single-layer cobaltates. Measurements of Co $L_3$-edge resonant inelastic X-ray scattering reveal the $t_{2g}$ electronic structure of Co for hole-doped La$_{2-x}$Sr$_x$CoO$_4$ ($x$ = 0.5, 0.7 and 0.8). As the Sr-doping $x$ increases, the tetragonal splitting of the $t_{2g}$ states of high-spin Co$^{2+}$ decreases, whereas that of low-spin Co$^{3+}$ increases and the fraction of high-spin Co$^{3+}$ increases. The results enable us to clarify the origin of the change of magnetic anisotropy and in-plane resistivity in a mixed-valence cobaltate caused by the interplay of spin-orbit coupling and tetragonal distortion.
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Submitted 13 August, 2021; v1 submitted 15 January, 2020;
originally announced January 2020.
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Electronic structure of the parent compound of superconducting infinite-layer nickelates
Authors:
M. Hepting,
D. Li,
C. J. Jia,
H. Lu,
E. Paris,
Y. Tseng,
X. Feng,
M. Osada,
E. Been,
Y. Hikita,
Y. -D. Chuang,
Z. Hussain,
K. J. Zhou,
A. Nag,
M. Garcia-Fernandez,
M. Rossi,
H. Y. Huang,
D. J. Huang,
Z. X. Shen,
T. Schmitt,
H. Y. Hwang,
B. Moritz,
J. Zaanen,
T. P. Devereaux,
W. S. Lee
Abstract:
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 cuprate…
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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.
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Submitted 5 September, 2019;
originally announced September 2019.
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Coulomb correlations intertwined with spin and orbital excitations in LaCoO$_3$
Authors:
K. Tomiyasu,
J. Okamoto,
H. Y. Huang,
Z. Y. Chen,
E. P. Sinaga,
W. B. Wu,
Y. Y. Chu,
A. Singh,
R. -P. Wang,
F. M. F. de Groot,
A. Chainani,
S. Ishihara,
C. T. Chen,
D. J. Huang
Abstract:
We carried out temperature-dependent (20 - 550 K) measurements of resonant inelastic X-ray scattering on LaCoO$_3$ to investigate the evolution of its electronic structure across the spin-state crossover. In combination with charge-transfer multiplet calculations, we accurately quantized the renormalized crystal-field excitation energies and spin-state populations. We show that the screening of th…
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We carried out temperature-dependent (20 - 550 K) measurements of resonant inelastic X-ray scattering on LaCoO$_3$ to investigate the evolution of its electronic structure across the spin-state crossover. In combination with charge-transfer multiplet calculations, we accurately quantized the renormalized crystal-field excitation energies and spin-state populations. We show that the screening of the on-site Coulomb interaction of 3d electrons is orbital selective and coupled to the spin-state crossover in LaCoO$_3$. The results establish that the gradual spin-state crossover is associated with a relative change of Coulomb energy versus bandwidth, leading to a Mott-type insulator-to-metal transition.
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Submitted 15 August, 2017;
originally announced August 2017.
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Jahn-Teller distortion driven magnetic polarons in magnetite
Authors:
H. Y. Huang,
Z. Y. Chen,
R. -P. Wang,
F. M. F. de Groot,
W. B. Wu,
J. Okamoto,
A. Chainani,
J. -S. Zhou,
H. -T. Jeng,
G. Y. Guo,
Je-Geun Park,
L. H. Tjeng,
C. T. Chen,
D. J. Huang
Abstract:
The first known magnetic mineral, magnetite (Fe$_3$O$_4$), has unusual properties which have fascinated mankind for centuries; it undergoes the Verwey transition at $T_{\rm V}$ $\sim$120 K with an abrupt change in structure and electrical conductivity. The mechanism of the Verwey transition however remains contentious. Here we use resonant inelastic X-ray scattering (RIXS) over a wide temperature…
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The first known magnetic mineral, magnetite (Fe$_3$O$_4$), has unusual properties which have fascinated mankind for centuries; it undergoes the Verwey transition at $T_{\rm V}$ $\sim$120 K with an abrupt change in structure and electrical conductivity. The mechanism of the Verwey transition however remains contentious. Here we use resonant inelastic X-ray scattering (RIXS) over a wide temperature range across the Verwey transition to identify and separate out the magnetic excitations derived from nominal Fe$^{2+}$ and Fe$^{3+}$ states. Comparison of the RIXS results with crystal-field multiplet calculations shows that the spin-orbital $dd$ excitons of the Fe$^{2+}$ sites arise from a tetragonal Jahn-Teller active polaronic distortion of the Fe$^{2+}$O$_6$ octahedra. These low-energy excitations, which get weakened for temperatures above 350 K but persist at least up to 550 K, are distinct from optical excitations and best explained as magnetic polarons.
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Submitted 13 August, 2016; v1 submitted 25 December, 2015;
originally announced December 2015.
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Raman and fluorescence characteristics of resonant inelastic X-ray scattering from doped superconducting cuprates
Authors:
H. Y. Huang,
C. J. Jia,
Z. Y. Chen,
K. Wohlfeld,
B. Moritz,
T. P. Devereaux,
W. B. Wu,
J. Okamoto,
W. S. Lee,
M. Hashimoto,
Y. He,
Z. X. Shen,
Y. Yoshida,
H. Eisaki,
C. Y. Mou,
C. T. Chen,
D. J. Huang
Abstract:
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 Rama…
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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.
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Submitted 28 October, 2015;
originally announced October 2015.
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New sum rule identities and duality relation for the Potts $n$-point correlation function
Authors:
F. Y. Wu,
H. Y. Huang
Abstract:
It is shown that certain sum rule identities exist which relate correlation functions for $n$ Potts spins on the boundary of a planar lattice for $n\geq 4$. Explicit expressions of the identities are obtained for $n=4,5$. It is also shown that the identities provide the missing link needed for a complete determination of the duality relation for the $n$-point correlation function. The $n=4$ dual…
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It is shown that certain sum rule identities exist which relate correlation functions for $n$ Potts spins on the boundary of a planar lattice for $n\geq 4$. Explicit expressions of the identities are obtained for $n=4,5$. It is also shown that the identities provide the missing link needed for a complete determination of the duality relation for the $n$-point correlation function. The $n=4$ duality relation is obtained explicitly. More generally we deduce the number of correlation identities for any $n$ as well as an inversion relation and a conjecture on the general form of the duality relation.
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Submitted 25 June, 1997;
originally announced June 1997.
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Lattice Statistics in Three Dimensions: Exact Solution of Layered Dimer and Layered Domain Wall Models
Authors:
V. Popkov,
Doochul Kim,
H. Y. Huang,
F. Y. Wu
Abstract:
Exact analyses are given for two three-dimensional lattice systems: A system of close-packed dimers placed in layers of honeycomb lattices and a layered triangular-lattice interacting domain wall model, both with nontrivial interlayer interactions. We show that both models are equivalent to a 5-vertex model on the square lattice with interlayer vertex-vertex interactions. Using the method of Bet…
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Exact analyses are given for two three-dimensional lattice systems: A system of close-packed dimers placed in layers of honeycomb lattices and a layered triangular-lattice interacting domain wall model, both with nontrivial interlayer interactions. We show that both models are equivalent to a 5-vertex model on the square lattice with interlayer vertex-vertex interactions. Using the method of Bethe ansatz, a closed-form expression for the free energy is obtained and analyzed. We deduce the exact phase diagram and determine the nature of the phase transitions as a function of the strength of the interlayer interaction.
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Submitted 6 March, 1997;
originally announced March 1997.
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Exact Solution of a Three-Dimensional Dimer System
Authors:
H. Y. Huang,
V. Popkov,
F. Y. Wu
Abstract:
We consider a three-dimensional lattice model consisting of layers of vertex models coupled with interlayer interactions. For a particular non-trivial interlayer interaction between charge-conserving vertex models and using a transfer matrix approach, we show that the eigenvalues and eigenvectors of the transfer matrix are related to those of the two-dimensional vertex model. The result is appli…
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We consider a three-dimensional lattice model consisting of layers of vertex models coupled with interlayer interactions. For a particular non-trivial interlayer interaction between charge-conserving vertex models and using a transfer matrix approach, we show that the eigenvalues and eigenvectors of the transfer matrix are related to those of the two-dimensional vertex model. The result is applied to analyze the phase transitions in a realistic three-dimensional dimer system.
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Submitted 25 October, 1996;
originally announced October 1996.
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Interacting dimers on the honeycomb lattice: An exact solution of the five-vertex model
Authors:
H. Y. Huang,
F. Y. Wu,
H. Kunz,
D. Kim
Abstract:
The problem of close-packed dimers on the honeycomb lattice was solved by Kasteleyn in 1963. Here we extend the solution to include interactions between neighboring dimers in two spatial lattice directions. The solution is obtained by using the method of Bethe ansatz and by converting the dimer problem into a five-vertex problem. The complete phase diagram is obtained and it is found that a new…
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The problem of close-packed dimers on the honeycomb lattice was solved by Kasteleyn in 1963. Here we extend the solution to include interactions between neighboring dimers in two spatial lattice directions. The solution is obtained by using the method of Bethe ansatz and by converting the dimer problem into a five-vertex problem. The complete phase diagram is obtained and it is found that a new frozen phase, in which the attracting dimers prevail, arises when the interaction is attractive. For repulsive dimer interactions a new first-order line separating two frozen phases occurs. The transitions are continuous and the critical behavior in the disorder regime is found to be the same as in the case of noninteracting dimers characterized by a specific heat exponent $\a=1/2$.
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Submitted 29 October, 1995;
originally announced October 1995.
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A Soluble Free-Fermion Model in d Dimensions
Authors:
F. Y. Wu,
H. Y. Huang
Abstract:
We consider a vertex model in d dimensions characterized by lines which run in a preferred direction. We show that this vertex model is soluble if the weights of vertices with intersecting lines are given by a free-fermion condition, and that a fugacity -1 is associated to each loop of lines. The solution is obtained by mapping the model into a dimer problem and by evaluating a Pfaffian. We also…
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We consider a vertex model in d dimensions characterized by lines which run in a preferred direction. We show that this vertex model is soluble if the weights of vertices with intersecting lines are given by a free-fermion condition, and that a fugacity -1 is associated to each loop of lines. The solution is obtained by mapping the model into a dimer problem and by evaluating a Pfaffian. We also determine the critical point and the singular behavior of the free energy.
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Submitted 9 December, 1994; v1 submitted 5 December, 1994;
originally announced December 1994.