I21-Resonant Inelastic X-ray Scattering (RIXS)
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Zubia
Hasan
,
Grace A.
Pan
,
Harrison
Labollita
,
Austin
Kaczmarek
,
Suk Hyun
Sung
,
Shekhar
Sharma
,
Purnima P.
Balakrishnan
,
Edward
Mercer
,
Vivek
Bhartiya
,
Alpha T.
N'Diaye
,
Zaher
Salman
,
Thomas
Prokscha
,
Andreas
Suter
,
Alexander J.
Grutter
,
Mirian
Garcia-Fernandez
,
Ke-Jin
Zhou
,
Jonathan
Pelliciari
,
Valentina
Bisogni
,
Ismail
El Baggari
,
Darrell G.
Schlom
,
Matthew R.
Barone
,
Charles M.
Brooks
,
Katja C.
Nowack
,
Antia S.
Botana
,
Brendan D.
Faeth
,
Alberto
De La Torre
,
Julia A.
Mundy
Diamond Proposal Number(s):
[34236]
Open Access
Abstract: 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 LiB2O4 materials. On the B-site frustrated pyrochlore sublattice, the interplay of correlated metallic behavior and charge frustration leads to a superconducting state in LiTi2O4 and heavy fermion behavior in LiV2O4. To date, however, LiTi2O4 has primarily been understood as a conventional BCS superconductor despite a lattice structure that could host more exotic ground states. Here, we present a multimodal investigation of LiTi2O4, 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 LiTi2O4 from other superconducting titanates, suggesting an unconventional origin to superconductivity in LiTi2O4. 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.
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Jan 2026
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I21-Resonant Inelastic X-ray Scattering (RIXS)
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Diamond Proposal Number(s):
[36210]
Open Access
Abstract: Quasiparticles describe collective excitations in many-body systems, and their symmetry classification is of fundamental importance for physical processes such as excited states, transport phenomena, and phase transitions. Recent studies have introduced chirality as an additional degree of freedom in condensed matter physics, leading to a range of novel phenomena. Among these, chiral phonons are of special interest because they carry angular momentum and therefore intrinsically break time reversal symmetry, which non-trivially bridges the spin system with the lattice. Here, we directly prove the presence of chiral phonons in a prototypical polar LiNbO3 crystal. Our demonstration of chiral phonons in a ferroelectric enables in-situ electrical control of momentum-dependent “magnetic” polarization with the reversible phonon handedness. This ferroic control of phonon chirality has substantial potential in the emerging field of chiral phononics, particularly along the associated control of its phonon angular momentum.
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Dec 2025
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I21-Resonant Inelastic X-ray Scattering (RIXS)
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Open Access
Abstract: Oxygen redox (OR) in Li1.2Ni0.13Co0.13Mn0.54O2 (LRNMC) and Na0.67Mg0.28Mn0.72O2 (NMMO) has been associated with the formation of embedded molecular O2 due to the appearance of their distinctive features in RIXS, while it is unclear whether OR also affects the oxygen left in the lattice. Here we use high-resolution oxygen K-edge resonant inelastic X-ray scattering (RIXS) at threshold excitation (527.5 – 529.5 eV) revealing lattice responses due to OR. We find that both cathodes show pronounced multiphonon progressions, which are either altered or activated upon charging. The first progression, with a fundamental energy loss ∼67-74 meV, matches the A1g lattice-oxygen mode observed by Raman spectroscopy, confirming its bulk origin. The second progression that exhibits a fundamental loss of ∼98 meV appears only at the highest state of charge and is resonant with the new pre-edge states at 527.5 eV. The latter mode emerges concurrently with the characteristic trapped-O2 RIXS signal and is strongly coupled to an occupied electronic band near the Fermi level, indicating that OR may not only contribute to the formation of molecular O2, but also perturbs lattice oxygen states, likely via polaron-forming oxidized lattice oxygen.
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Dec 2025
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I21-Resonant Inelastic X-ray Scattering (RIXS)
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D.
Takegami
,
T.
Aoyama
,
T.
Okauchi
,
T.
Yamaguchi
,
S.
Tippireddy
,
S.
Agrestini
,
Mirian
Garcia-Fernandez
,
T.
Mizokawa
,
K.
Ohgushi
,
Ke-Jin
Zhou
,
J.
Chaloupka
,
J.
Kuneš
,
A.
Hariki
,
H.
Suzuki
Diamond Proposal Number(s):
[35709]
Open Access
Abstract: X-ray magnetic circular dichroism provides a means to identify ferromagnetic, chiral, and altermagnetic orders via their time-reversal-symmetry (𝒯) breaking. However, the symmetry properties that govern circular dichroism (CD) in resonant inelastic x-ray scattering (RIXS) remain poorly understood. We show that, due to the inherent irreversibility of the RIXS process, RIXS-CD does not require 𝒯 breaking to be present, but reflects the change in unitary symmetries associated with magnetic ordering. Using the altermagnetic MnTe as a model system, we observe an azimuthal-angle dependent RIXS-CD signal in the magnon excitations. Our findings highlight the sensitivity of RIXS-CD to the relativistic symmetry in magnetic systems and its potential application as a probe of magnetic domains.
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Nov 2025
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I21-Resonant Inelastic X-ray Scattering (RIXS)
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Diamond Proposal Number(s):
[38040]
Open Access
Abstract: 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.
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Oct 2025
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I21-Resonant Inelastic X-ray Scattering (RIXS)
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Abstract: Mott-insulating 5d double perovskites (DPs) have recently emerged as strongly correlated electron systems of interest due to the novel multipolar physics they display. Key to understanding these properties is proper identification of the energy scales in the electronic Hamiltonian, for which resonant inelastic X-ray scattering (RIXS) is an ideal tool. In the A2MgReO6 (A = Ca, Sr, Ba) 5d1 DPs, Re L3 edge RIXS reveals that the 5d shell is split at a high level by the crystalline electric field (CEF) and at a low level by strong spin-orbit coupling (SOC). Unexpectedly, the SOC excitations are dressed by Jahn-Teller (JT) active phonon modes, implying the presence of a dynamic JT effect. This dynamic JT effect couples the electronic and lattice degrees of freedom, resulting in a spin-orbit-lattice entangled ground state. Vibronic RIXScalculations support these findings and estimate the dynamic JT effect to be one order of magnitude weaker than the SOC. Higher resolution O K edge RIXS measurements of the A2MgReO6 DPs are also presented, wherein the 5d1 ground state is probed via Re 5d - O 2p orbital hybridization. This higher resolution resolves the individual vibronic modes dressing the SOC excitations, and expanded temperature dependence measurements reveal systematic evolution of the dynamic JT effect. Significant enhancement of low energy phononic features is observed at the O K edge as predicted theoretically.Intermediate state effects are believed to imprint the spectra in O K edge RIXS due to the longer core-hole lifetime. In the 5d2 DPs Ba2YReO6 and Sr2CrReO6, Re L2 and L3 edge RIXS reveals that the 5d levels are split at a high level by the CEF as in the 5d1 case. The 5d2 and 5d1 cases diverge at lower energy where the 5d2 levels are split into several multiplets by the interplay of SOC and Hund’s coupling introduced by the presence of a second electron. Computational methods are used to successfully untangle the individual energy scales of the Hund’s and spin-orbit couplings. Differences between the L2 and L3 spectra reflective of dipole selection rules prove key to being able to unambiguously separate these energy scales.
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Oct 2025
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I10-Beamline for Advanced Dichroism - scattering
I21-Resonant Inelastic X-ray Scattering (RIXS)
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Andrey D.
Poletayev
,
Robert J.
Green
,
Jack E. N.
Swallow
,
Lijin
An
,
Leanne
Jones
,
Grant
Harris
,
Peter
Bencok
,
Ronny
Sutarto
,
Jonathon P.
Cottom
,
Benjamin J.
Morgan
,
Robert A.
House
,
Robert S.
Weatherup
,
M. Saiful
Islam
Diamond Proposal Number(s):
[33062, 30644]
Open Access
Abstract: Nickelate materials offer diverse functionalities for energy and computing applications. Lithium nickel oxide (LiNiO2) is an archetypal layered nickelate, but the electronic structure of this correlated material is not yet fully understood. Here we investigate the temperature-dependent speciation and spin dynamics of Ni ions in LiNiO2. Ab initio simulations predict that Ni ions disproportionate into three states, which dynamically interconvert and whose populations vary with temperature. These predictions are verified using x-ray absorption spectroscopy, x-ray magnetic circular dichroism, and resonant inelastic x-ray scattering at the Ni L3,2-edge. Charge-transfer multiplet calculations consistent with disproportionation reproduce all experimental features. Our results support a model of dynamic disproportionation that explains diverse physical observations of LiNiO2, including magnetometry, thermally activated electronic conduction, diffractometry, core-level spectroscopies, and the stability of ubiquitous antisite defects. This unified understanding of the material properties of LiNiO2 is important for applications of nickelate materials as battery cathodes, catalysts, and superconductors.
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Oct 2025
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I21-Resonant Inelastic X-ray Scattering (RIXS)
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L.
Martinelli
,
I.
Biało
,
X.
Hong
,
J.
Oppliger
,
C.
Lin
,
T,
Schaller
,
J.
Küspert
,
M. H.
Fischer
,
T.
Kurosawa
,
N.
Momono
,
M.
Oda
,
D. V.
Novikov
,
A.
Khadiev
,
E.
Weschke
,
J.
Choi
,
S.
Agrestini
,
Mirian
Garcia-Fernandez
,
Ke-Jin
Zhou
,
Q.
Wang
,
J.
Chang
Diamond Proposal Number(s):
[33512]
Open Access
Abstract: 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 fourfold 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 behavior and remains a possible source for the strange metal properties found in the normal state of cuprate superconductors.
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Jul 2025
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I21-Resonant Inelastic X-ray Scattering (RIXS)
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Daniel
Jost
,
Eder G.
Lomeli
,
Woo Jin
Kim
,
Emily M.
Been
,
Matteo
Rossi
,
Stefano
Agrestini
,
Ke-Jin
Zhou
,
Chunjing
Jia
,
Brian
Moritz
,
Zhi-Xun
Shen
,
Harold Y.
Hwang
,
Thomas P.
Devereaux
,
Wei-Sheng
Lee
Diamond Proposal Number(s):
[30402]
Open Access
Abstract: The layered cobaltate CaCoO2 exhibits a unique herringbone-like structure. Serving as a potential prototype for a new class of complex lattice patterns, we study the properties of CaCoO2 using X-ray absorption spectroscopy (XAS) and resonant inelastic X-ray scattering (RIXS). Our results reveal a significant inter-plane hybridization between the Ca 4s- and Co 3d- orbitals, leading to an inversion of the textbook orbital occupation of a square planar geometry. Further, our RIXS data reveal a strong low energy mode, with anomalous intensity modulations as a function of momentum transfer close to a quasi-static response. These findings indicate that the newly discovered herringbone structure exhibited in CaCoO2 may serve as a promising laboratory for the design of materials having strong electronic, orbital and lattice correlations.
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Jun 2025
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I21-Resonant Inelastic X-ray Scattering (RIXS)
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Karin
Von Arx
,
Pascal
Rothenbühler
,
Qisi
Wang
,
Leonardo
Martinelli
,
Jaewon
Choi
,
Mirian
Garcia-Fernandez
,
Stefano
Agrestini
,
Ke-Jin
Zhou
,
Antonio
Vecchione
,
Rosalba
Fittipaldi
,
Yasmine
Sassa
,
Mario
Cuoco
,
Filomena
Forte
,
Johan
Chang
Diamond Proposal Number(s):
[27638]
Open Access
Abstract: Multi-band Mott insulators with moderate spin-orbit and Hund’s coupling are key reference points for theoretical concept developments of correlated electron systems. The ruthenate Mott insulator Ca2RuO4 has therefore been intensively studied by spectroscopic probes. However, it has been challenging to resolve the fundamental excitations emerging from the hierarchy of electronic energy scales. Here we apply high resolution resonant inelastic x-ray scattering to probe deeper into the low-energy electronic excitations found in Ca2RuO4. In this fashion, we probe a series of spin-orbital excitations. By taking advantage of enhanced energy resolution, we probe a 40 meV mode through the oxygen K-edge. The polarization dependence of this low-energy excitations exposes a distinct orbital nature, originating from the interplay of spin-orbit coupling and octahedral rotations. Additionally, we discuss the role of magnetic correlations to describe the occurrence of excitations with amplitudes which are multiple of a given energy. Such direct determination of relevant electronic energy scales sharpens the target for theory developments of Mott insulators’ orbital degree of freedom.
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May 2025
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