I21-Resonant Inelastic X-ray Scattering (RIXS)
|
Xiaoyang
Chen
,
Wenliang
Zhang
,
Fei
Peng
,
Ting
Cui
,
Guangdi
Zhou
,
Zezhong
Li
,
Jaewon
Choi
,
Lizhi
Xu
,
Yiu-Fung
Chiu
,
Stefano
Agrestini
,
Sahil
Tippireddy
,
Haoliang
Huang
,
Heng
Wang
,
Xianfeng
Wu
,
Peng
Li
,
Jin-Feng
Jia
,
Mirian
Garcia-Fernandez
,
Yi
Lu
,
Er-Jia
Guo
,
Qi-Kun
Xue
,
Zhuoyu
Chen
,
Donglai
Feng
,
Ke-Jin
Zhou
Diamond Proposal Number(s):
[42637]
Open Access
Abstract: The recent discovery of Ruddlesden-Popper (RP) nickelate thin-film superconductors has opened a new frontier in unconventional superconductivity. Its realization requires both compressive epitaxial strain and highly oxidative growth conditions, yet the microscopic pathway from the parent phase to the superconducting phase remains elusive. Here, X-ray absorption spectra and resonant inelastic X-ray scattering are employed to track this evolution by independently tuning strain and oxygen content in (La,Pr)3Ni2O7 − δ thin films. We uncover a remarkable two-step narrative. First, signatures of delocalization emerge: Spectral weight transfers from a “Upper Hubbard”-like peak to the hole-like peak associated with O 2pz state, and in parallel, the initially localized Ni
orbital becomes more itinerant followed by the broadening and weakening of dd orbital excitations. Second, as itinerancy increases, long-range spin-density-wave (SDW) order is suppressed in both intensity and correlation length, indicating direct competition with superconductivity. Yet, short-range magnons persist: they become damped but their bandwidth stays unchanged. Our results paint a coherent picture that both strain and oxygenation drive the RP bilayer nickelates towards the superconducting instability, where the O 2pz and Ni
orbitals become delocalized. Concomitantly, the long-range magnetic order loses coherence and gets suppressed. These findings establish an orbital-selective route to RP nickelate superconductivity, in which the emergence and progressive delocalization of the interlayer
-2pz-
channel and the robust short-range magnons upon the melting of SDW order are prerequisites, providing strong constraints for theory and the roadmap for designing nickelate superconductors.
|
Aug 2026
|
|
|
|
Abstract: Taking the quadruple perovskite oxide CaCu3Fe2Os2O12 as an example, by performing both experimental sum rules and theoretical configuration interaction cluster calculations, we have investigated the spin and orbital configurations of all the transition metal cations, Cu, Fe, and Os, as well as their local microscopic physical parameters of crystal field, spin–orbit coupling (SOC), Coulomb potential, and hybridization. Specifically, we found that Os5+ (5d3) with a half-filled t2g orbital exhibits a large orbital moment on account of the mixing of t2g and eg orbitals, which can be ascribed to the strong SOC of the 5d elements. On the other hand, SOC of the Cu2+ (3d9) is markedly reduced, but is still nonnegligible compared to the crystal field 10Dq, leading to a finite orbital moment of Cu2+. This work provides a microscopic and element-selective perspective of the local environment of magnetic cations in complex compounds.
|
Aug 2026
|
|
I21-Resonant Inelastic X-ray Scattering (RIXS)
|
Diamond Proposal Number(s):
[24600, 30866]
Open Access
Abstract: The electron in a solid can be considered a bound state of the three independent, fundamental degrees of freedom creating quasiparticles: spinons, carrying the electron spin; plasmons, carrying the collective charge mode; and orbitons, carrying its orbital degree of freedom. These fundamental degrees of freedom could form ordering states in which dynamics or collective motions could occur and manifest as low-energy excitations. The exotic properties that appear in the materials exhibiting these electronic orderings are associated with these low-energy excitations. Although the orbital order (OO) and its coupling to the spin system creates very interesting phenomena, the microscopic origin of OO has been much less explored than other electronic properties as it is very difficult to directly access experimentally. Due to the recent improvement in energy resolution and flux, soft-x-ray resonant inelastic scattering (RIXS) allows for a reexamination of orbital excitations in manganites. Here, we present a study of low-energy excitations in half doped 𝐴-site ordered SmBaMn2O6 through a combination of RIXS and soft-x-ray resonant elastic scattering measurements. We confirm the existence of OO at 𝐪 = (0.25, 0.25, 0) and find various low-energy excitations below 200 meV. While several excitations can be assigned to be of magnetic and phononic origin, a group of excitations between 80 and 200 meV show a temperature dependence closely following that of the OO, making them possible candidates for orbitons.
|
Jun 2026
|
|
I21-Resonant Inelastic X-ray Scattering (RIXS)
|
Grace A.
Pan
,
Dan Ferenc
Segedin
,
Sophia F. R.
Tenhuisen
,
Lopa
Bhatt
,
Harrison
Labollita
,
Abigail Y.
Jiang
,
Qi
Song
,
Ari B.
Turkiewicz
,
Denitsa R.
Baykusheva
,
Abhishek
Nag
,
Stefano
Agrestini
,
Ke-Jin
Zhou
,
Jonathan
Pelliciari
,
Valentina
Bisogni
,
Hua
Zhou
,
Mark P. M.
Dean
,
Hanjong
Paik
,
David A.
Muller
,
Lena F.
Kourkoutis
,
Charles M.
Brooks
,
Matteo
Mitrano
,
Antia S.
Botana
,
Berit H.
Goodge
,
Julia A.
Mundy
Diamond Proposal Number(s):
[27484]
Abstract: The discovery of superconductivity in square-planar nickelates has offered a rich materials platform to explore the origins of high-temperature superconductivity. However, experimental investigations have largely been limited to the infinite-layer RNiO2 (R, rare earth) nickelates. We constructed a phase diagram of multilayer square-planar Ndn+1NinO2n+2 compounds and found signatures of superconductivity for dimensionality n = 4 to 8. Upon decreasing n, the superconducting anisotropy evolves owing to 4f electron effects, and electronic structure characteristics approach cuprate-like behavior. Magnetic fluctuations persist from within the superconducting regime and into the overdoped, nonsuperconducting regime. The superconducting regime overlaps with that of chemically doped infinite-layer nickelates, demonstrating underlying commonalities as well as differences across varying structural realizations of square-planar nickelates. Our work establishes this layered template for creating new nickel-based superconductors.
|
Jun 2026
|
|
I21-Resonant Inelastic X-ray Scattering (RIXS)
|
Kunhao
Li
,
Qizhi
Li
,
Changwei
Zou
,
Jaewon
Choi
,
Chaohui
Yin
,
Mirian
Garcia-Fernandez
,
Stefano
Agrestini
,
Shilong
Zhang
,
Chengtian
Lin
,
Xingjiang
Zhou
,
Ke-Jin
Zhou
,
Yi
Lu
,
Yingying
Peng
Diamond Proposal Number(s):
[30361]
Abstract: The superconducting gap is a characteristic feature of high-𝑇c superconductors and provides crucial information on the pairing mechanism underlying high-temperature superconductivity. Here, we employ high-resolution resonant inelastic x-ray scattering (RIXS) at the Cu 𝐿3 edge to investigate the superconducting gap in the overdoped cuprate Bi2Sr2Ca2Cu3O10+𝛿 (𝑇c=107K). By analyzing antisymmetrized, temperature-dependent RIXS spectra over a range of in-plane momentum transfers, we observe a clear suppression of low-energy spectral weight below 𝑇c, indicative of superconducting-gap formation. This suppression is most pronounced at small momentum transfers [
| | |
𝒒∥
| | |
≤0.18 r.l.u. (reciprocal lattice units)] and corresponds to a gap size of approximately 2Δ0∼130 meV. Comparison with theoretical calculations of the momentum-dependent charge susceptibility supports a 𝑑-wave symmetry of the superconducting gap, while an isotropic 𝑠-wave gap fails to reproduce key experimental features. These findings establish RIXS as a powerful, bulk-sensitive probe of superconducting-gap symmetry and highlight its utility for studying materials beyond the reach of surface-sensitive techniques such as ARPES and STM.
|
Jun 2026
|
|
I21-Resonant Inelastic X-ray Scattering (RIXS)
|
Diamond Proposal Number(s):
[29150]
Open Access
Abstract: Cuprate superconductors show various collective charge correlations that are intimately connected with their electronic properties. In particular, charge order in the form of an incommensurate charge density wave (CDW) order with an in-plane wave vector 𝛿CDW≈0.23–0.35 reciprocal lattice units appears to be universally present. In addition to CDW, dynamic charge density fluctuations (CDFs) are also present with wave vectors comparable to 𝛿CDW. CDFs are present up to ≈300K and have relatively short correlation lengths of 𝜉≈20Å. Here we use Cu-𝐿3 and O-𝐾 resonant inelastic x-ray scattering (RIXS) to study the doping dependence of CDW and CDFs in La2−𝑥Sr𝑥CuO4. We fit our data with (quasi)elastic peaks resulting from the CDW and up to four inelastic modes associated with oxygen phonons that can be strongly coupled to the CDFs. Our analysis allows us to separate the charge correlations into three components: the CDW with wave vector 𝛿4𝑎-CDW≈0.24 and two CDF components with 𝛿4𝑎-CDF≈0.24 and 𝛿3𝑎-CDF≈0.30. We find that for 𝑇≈𝑇𝑐 the CDW coexists with the CDFs for dopings near 𝑥=𝑝≈1/8. The 4𝑎-CDW disappears beyond 𝑥=0.16 and the 4𝑎-CDF beyond 𝑥=0.19, leaving only a weak 3𝑎-CDF at the highest doping studied, 𝑥=0.22. Our data suggest that low-energy charge fluctuations exist up to doping 𝑥=0.19=𝑝★, where the pseudogap disappears; however, we find no evidence that they are associated with a quantum critical point.
|
May 2026
|
|
I21-Resonant Inelastic X-ray Scattering (RIXS)
|
Ke-Jin
Zhou
,
Qiushi
Huang
,
Mirian
Garcia-Fernandez
,
Yeqi
Zhuang
,
Stefano
Agrestini
,
Shengyou
Wen
,
Thomas
Rice
,
Sahil
Tippireddy
,
Jaewon
Choi
,
Andrew
Walters
,
Igor V.
Kozhevnikov
,
Zhe
Zhang
,
Runze
Qi
,
Zhong
Zhang
,
Hongchang
Wang
,
Zhanshan
Wang
Open Access
Abstract: Resonant inelastic X-ray scattering (RIXS) is a photon-in/photon-out spectroscopic technique which has become increasingly important for the condensed matter physics community. The development of the RIXS instrumentation in soft X-ray and hard X-ray range facilitated the research in 3d and 5d transition metal (TM)-based materials, respectively. However, the tender X-ray (2000–3000 eV) RIXS covering most of 4d TM-based materials severely falls behind due to the lack of high-performance energy dispersive optics. Here, we demonstrate the design and fabrication of a laterally graded multilayer grating (MLG) optics for the establishment of the tender RIXS at the I21 RIXS beamline in Diamond Light Source. The successful implementation of the MLG boosts the photon flux by more than an order of magnitude at the Sulfur K-edge (2475 eV) and the Ru L3-edge (2838 eV) in comparison to the solution of a single-layer coated grating (SLG). More importantly, MLG retains the high energy resolution of the SLG design (~10,000) and works continuously across the full range of 2000–3000 eV. It renders the I21 beamline as the very first RIXS facility in the world that covers both soft and tender X-rays (280–3000 eV) using a grating-based spectrometer for a wide range of science applications.
|
Jan 2026
|
|
Optics
|
Arindam
Majhi
,
Wadwan
Singhapong
,
Wai Jue
Tan
,
Andrey
Sokolov
,
Stefano
Agrestini
,
Mirian
Garcia-Fernandez
,
Ke-Jin
Zhou
,
Andrew C.
Walters
,
Chris
Bowen
,
Alexander J. G.
Lunt
,
Hongchang
Wang
,
Kawal J.
Sawhney
Open Access
Abstract: Laterally graded multilayer optics play an important role in advanced X-ray applications, enabling precise control of beam properties for spectroscopic and focusing techniques. The Multilayer Deposition System (MDS) at Diamond Light Source (DLS) has demonstrated its ability to fabricate highly precise laterally graded X-ray optics. Developing such optics is challenging due to stringent requirements for precise lateral thickness variations and sagittal uniformity, achieved through optimized substrate speed profiles and advanced mask design. This study presents a comprehensive investigation into the design, fabrication, and characterization of laterally graded multilayers. An adjustable mask design improves sagittal uniformity and reduces optimization times. The structural and optical performance of the multilayers is evaluated, confirming their suitability for synchrotron applications. Two types of laterally graded multilayers were developed: one with a constant lateral gradient (0.005 nm/mm) for O-K edge polarizers, achieving sagittal thickness variations of approximately 0.3–0.4% across an 80 mm substrate, and another featuring a strong variable gradient from 0.037 to 0.112 nm/mm, designed to match the elliptical periodicity profile. The constant gradient multilayer polarizer has been successfully implemented on the state-of-the-art I21 beamline at DLS, highlighting the MDS's role in producing next-generation X-ray optics that meet the stringent demands of synchrotron beamlines.
|
Jan 2026
|
|
I21-Resonant Inelastic X-ray Scattering (RIXS)
|
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.
|
Nov 2025
|
|
I21-Resonant Inelastic X-ray Scattering (RIXS)
|
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.
|
Oct 2025
|
|
