I21-Resonant Inelastic X-ray Scattering (RIXS)
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Open Access
Abstract: A photon carrying one unit of angular momentum can change the spin angular momentum of a magnetic system with one unit (ΔMs = ±1) at most. This implies that a two-photon scattering process can manipulate the spin angular momentum of the magnetic system with a maximum of two units. Herein we describe a triple-magnon excitation in α-Fe2O3, which contradicts this conventional wisdom that only 1- and 2-magnon excitations are possible in a resonant inelastic X-ray scattering experiment. We observe an excitation at exactly three times the magnon energy, along with additional excitations at four and five times the magnon energy, suggesting quadruple and quintuple-magnons as well. Guided by theoretical calculations, we reveal how a two-photon scattering process can create exotic higher-rank magnons and the relevance of these quasiparticles for magnon-based applications.
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May 2023
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I21-Resonant Inelastic X-ray Scattering (RIXS)
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Andrea
Amorese
,
Philipp
Hansmann
,
Andrea
Marino
,
Peter
Körner
,
Thomas
Willers
,
Andrew
Walters
,
Ke-Jin
Zhou
,
Kurt
Kummer
,
Nicholas B.
Brookes
,
Hong-Ji
Lin
,
Chien-Te
Chen
,
Pascal
Lejay
,
Maurits W.
Haverkort
,
Liu Hao
Tjeng
,
Andrea
Severing
Diamond Proposal Number(s):
[18447]
Open Access
Abstract: We investigated the electronic structure of the enigmatic
CeRh
3
B
2
using resonant inelastic scattering and x-ray absorption spectroscopy in combination with ab initio density functional calculations. We find that the
Rh
4
d
states are irrelevant for the high-temperature ferromagnetism and the Kondo effect. We also find that the
Ce
4
f
crystal-field strength is too small to explain the strong reduction of the Ce magnetic moment. The data revealed instead the presence of two different active
Ce
4
f
orbitals, with each coupling selectively to different bands in
CeRh
3
B
2
. The intersite hybridization of the
∣
∣
J
=
5
2
,
J
z
=
±
1
2
⟩
crystal-field state and
Ce
5
d
band combined with the intrasite
Ce
4
f
–
5
d
exchange creates the strong ferromagnetism, while hybridization between the
∣
∣
J
=
5
2
,
J
z
=
±
5
2
⟩
and the B
s
p
in the
a
b
-plane contributes to the Kondo interaction, which causes the moment reduction. This orbital selective coupling explains the unique and seemingly contradictory properties of
CeRh
3
B
2
.
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Mar 2023
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I21-Resonant Inelastic X-ray Scattering (RIXS)
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Xiang
Ding
,
Charles C.
Tam
,
Xuelei
Sui
,
Yan
Zhao
,
Minghui
Xu
,
Jaewon
Choi
,
Huaqian
Leng
,
Ji
Zhang
,
Mei
Wu
,
Haiyan
Xiao
,
Xiaotao
Zu
,
Mirian
Garcia-Fernandez
,
Stefano
Agrestini
,
Xiaoqiang
Wu
,
Qingyuan
Wang
,
Peng
Gao
,
Sean
Li
,
Bing
Huang
,
Ke-Jin
Zhou
,
Liang
Qiao
Diamond Proposal Number(s):
[30296]
Abstract: The newly discovered nickelate superconductors so far only exist in epitaxial thin films synthesized by a topotactic reaction with metal hydrides1. This method changes the nickelates from the perovskite to an infinite-layer structure by deintercalation of apical oxygens1,2,3. Such a chemical reaction may introduce hydrogen (H), influencing the physical properties of the end materials4,5,6,7,8,9. Unfortunately, H is insensitive to most characterization techniques and is difficult to detect because of its light weight. Here, in optimally Sr doped Nd0.8Sr0.2NiO2H epitaxial films, secondary-ion mass spectroscopy shows abundant H existing in the form of Nd0.8Sr0.2NiO2Hx (x ≅ 0.2–0.5). Zero resistivity is found within a very narrow H-doping window of 0.22 ≤ x ≤ 0.28, showing unequivocally the critical role of H in superconductivity. Resonant inelastic X-ray scattering demonstrates the existence of itinerant interstitial s (IIS) orbitals originating from apical oxygen deintercalation. Density functional theory calculations show that electronegative H– occupies the apical oxygen sites annihilating IIS orbitals, reducing the IIS–Ni 3d orbital hybridization. This leads the electronic structure of H-doped Nd0.8Sr0.2NiO2Hx to be more two-dimensional-like, which might be relevant for the observed superconductivity. We highlight that H is an important ingredient for superconductivity in epitaxial infinite-layer nickelates.
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Mar 2023
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I21-Resonant Inelastic X-ray Scattering (RIXS)
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Abstract: Spinel oxides are well-known functional materials but rarely show superconductivity. Recently, emergent superconductivity was discovered in
MgTi
2
O
4
, which is attributed to the increase of electron doping and the suppression of orbital order. Here, we utilized Ti
L
-edge resonant inelastic x-ray scattering to study the orbital excitations in superconducting (SC) and insulating
MgTi
2
O
4
films. We find that the spectral weight of orbital excitations is enhanced and the energy of
t
2
g
intraband excitation is softened in the SC film compared to the insulating one, suggesting higher electron doping and a suppressed orbital order gap in the SC sample. These observations were further supported by our multiplet calculations using the minimal two-site model. Our results provide spectroscopic evidence for the competition between orbital order and superconductivity in
MgTi
2
O
4
and shed light on searching for novel superconductors in spinel oxides.
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Mar 2023
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I21-Resonant Inelastic X-ray Scattering (RIXS)
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Robert A.
House
,
Gregory J.
Rees
,
Kit
Mccoll
,
John-Joseph
Marie
,
Mirian
Garcia-Fernandez
,
Abhishek
Nag
,
Ke-Jin
Zhou
,
Simon
Cassidy
,
Benjamin J.
Morgan
,
M.
Saiful Islam
,
Peter G.
Bruce
Diamond Proposal Number(s):
[25589]
Abstract: Oxide ions in transition metal oxide cathodes can store charge at high voltage offering a route towards higher energy density batteries. However, upon charging these cathodes, the oxidized oxide ions condense to form molecular O2 trapped in the material. Consequently, the discharge voltage is much lower than charge, leading to undesirable voltage hysteresis. Here we capture the nature of the electron holes on O2− before O2 formation by exploiting the suppressed transition metal rearrangement in ribbon-ordered Na0.6[Li0.2Mn0.8]O2. We show that the electron holes formed are delocalized across the oxide ions coordinated to two Mn (O–Mn2) arranged in ribbons in the transition metal layers. Furthermore, we track these delocalized hole states as they gradually localize in the structure in the form of trapped molecular O2 over a period of days. Establishing the nature of hole states on oxide ions is important if truly reversible high-voltage O-redox cathodes are to be realized.
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Feb 2023
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I21-Resonant Inelastic X-ray Scattering (RIXS)
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Abhishek
Nag
,
Yiran
Peng
,
Jiemin
Li
,
Stefano
Agrestini
,
Hannah C.
Robarts
,
Mirian
Garcia-Fernandez
,
Andrew C.
Walters
,
Qi
Wang
,
Qiangwei
Yin
,
Hechang
Lei
,
Zhiping
Yin
,
Ke-Jin
Zhou
Diamond Proposal Number(s):
[27905]
Open Access
Abstract: Among condensed matter systems, Mott insulators exhibit diverse properties that emerge from electronic correlations. In itinerant metals, correlations are usually weak, but can also be enhanced via geometrical confinement of electrons, that manifest as ‘flat’ dispersionless electronic bands. In the fast developing field of topological materials, which includes Dirac and Weyl semimetals, flat bands are one of the important components that can result in unusual magnetic and transport behaviour. To date, characterisation of flat bands and their magnetism is scarce, hindering the design of novel materials. Here, we investigate the ferromagnetic Kagomé semimetal Co3Sn2S2 using resonant inelastic X-ray scattering. Remarkably, nearly non-dispersive Stoner spin excitation peaks are observed, sharply contrasting with the featureless Stoner continuum expected in conventional ferromagnetic metals. Our band structure and dynamic spin susceptibility calculations, and thermal evolution of the excitations, confirm the nearly non-dispersive Stoner excitations as unique signatures of correlations and spin-polarized electronic flat bands in Co3Sn2S2. These observations serve as a cornerstone for further exploration of band-induced symmetry-breaking orders in topological materials.
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Nov 2022
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I21-Resonant Inelastic X-ray Scattering (RIXS)
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Haiyu
Lu
,
Makoto
Hashimoto
,
Su-Di
Chen
,
Shigeyuki
Ishida
,
Dongjoon
Song
,
Hiroshi
Eisaki
,
Abhishek
Nag
,
Mirian
Garcia-Fernandez
,
Riccardo
Arpaia
,
Giacomo
Ghiringhelli
,
Lucio
Braicovich
,
Jan
Zaanen
,
Brian
Moritz
,
Kurt
Kummer
,
Nicholas B.
Brookes
,
Ke-Jin
Zhou
,
Zhi-Xun
Shen
,
Thomas P.
Devereaux
,
Wei-Sheng
Lee
Diamond Proposal Number(s):
[22009]
Abstract: Identifying quantum critical points (QCPs) and their associated fluctuations may hold the key to unraveling the unusual electronic phenomena observed in cuprate superconductors. Recently, signatures of quantum fluctuations associated with charge order (CO) have been inferred from the anomalous enhancement of CO excitations that accompany the reduction of the CO order parameter in the superconducting state. To gain more insight into the interplay between CO and superconductivity, here we investigate the doping dependence of this phenomenon throughout the Bi-2212 cuprate phase diagram using resonant inelastic x-ray scattering (RIXS) at the Cu
L
3
edge. As doping increases, the CO wave vector decreases, saturating near a commensurate value of 0.25 reciprocal lattice unit beyond a characteristic doping
p
c
, where the correlation length becomes shorter than the apparent periodicity (
4
a
0
). Such behavior is indicative of the fluctuating nature of the CO; the proliferation of CO excitations in the superconducting state also appears strongest at
p
c
, consistent with expected behavior at a CO QCP. Intriguingly,
p
c
appears to be near optimal doping, where the superconducting transition temperature
T
c
is maximal.
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Oct 2022
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I21-Resonant Inelastic X-ray Scattering (RIXS)
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U.
Kumar
,
A.
Nag
,
J.
Li
,
H. C.
Robarts
,
A. C.
Walters
,
M.
Garcia-Fernandez
,
R.
Saint-Martin
,
A.
Revcolevschi
,
J.
Schlappa
,
T.
Schmitt
,
Steven
Johnston
,
K.-J.
Zhou
Diamond Proposal Number(s):
[21184]
Abstract: Resonant inelastic x-ray scattering (RIXS) is an evolving tool for investigating the spin dynamics of strongly correlated materials, which complements inelastic neutron scattering. In isotropic spin-
1
2
Heisenberg antiferromagnetic (HAFM) spin chains, both techniques have observed non-spin-conserving (NSC) excitations confined to the two-spinon phase space. However, a recent O
K
-edge RIXS study of the one-dimensional HAFM
Sr
2
CuO
3
observed spin-conserving (SC) four-spinon excitations outside the two-spinon phase space. Here, we demonstrate that analogous four-spinon excitations can also be accessed at the Cu
L
3
edge in the related material
SrCuO
2
. Through detailed modeling, we establish that these excitations appear in both the SC and NSC channels of the Cu
L
3
edge, and are only captured by higher-order terms in the ultrashort core-hole lifetime expansion. Since these terms encode information about spin-spin correlations extending beyond nearest neighbors, our results offer different possibilities for studying nonlocal spin correlations in quantum magnets.
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Aug 2022
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I21-Resonant Inelastic X-ray Scattering (RIXS)
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Charles C.
Tam
,
Jaewon
Choi
,
Xiang
Ding
,
Stefano
Agrestini
,
Abhishek
Nag
,
Mei
Wu
,
Bing
Huang
,
Huiqian
Luo
,
Peng
Gao
,
Mirian
Garcia-Fernandez
,
Liang
Qiao
,
Ke-Jin
Zhou
Diamond Proposal Number(s):
[30296]
Abstract: In materials science, much effort has been devoted to the reproduction of superconductivity in chemical compositions, analogous to cuprate superconductors since their discovery over 30 years ago. This approach was recently successful in realising superconductivity in infinite-layer nickelates1,2,3,4,5,6. Although differing from cuprates in electronic and magnetic properties, strong Coulomb interactions suggest that infinite-layer nickelates have a propensity towards various symmetry-breaking orders that populate cuprates7,8,9,10. Here we report the observation of charge density waves (CDWs) in infinite-layer NdNiO2 films using Ni L3 resonant X-ray scattering. Remarkably, CDWs form in Nd 5d and Ni 3d orbitals at the same commensurate wavevector (0.333, 0) reciprocal lattice units, with non-negligible out-of-plane dependence and an in-plane correlation length of up to ~60 Å. Spectroscopic studies reveal a strong connection between CDWs and Nd 5d–Ni 3d orbital hybridization. Upon entering the superconducting state at 20% Sr doping, the CDWs disappear. Our work demonstrates the existence of CDWs in infinite-layer nickelates with a multiorbital character distinct from cuprates, which establishes their low-energy physics.
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Aug 2022
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I21-Resonant Inelastic X-ray Scattering (RIXS)
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Matteo
Rossi
,
Motoki
Osada
,
Jaewon
Choi
,
Stefano
Agrestini
,
Daniel
Jost
,
Yonghun
Lee
,
Haiyu
Lu
,
Bai Yang
Wang
,
Kyuho
Lee
,
Abhishek
Nag
,
Yi-De
Chuang
,
Cheng-Tai
Kuo
,
Sang-Jun
Lee
,
Brian
Moritz
,
Thomas P.
Devereaux
,
Zhi-Xun
Shen
,
Jun-Sik
Lee
,
Ke-Jin
Zhou
,
Harold Y.
Hwang
,
Wei-Sheng
Lee
Diamond Proposal Number(s):
[25598, 27558]
Abstract: A defining signature of strongly correlated electronic systems is a rich phase diagram, which consists of multiple broken symmetries, such as magnetism, superconductivity and charge order1,2. In the recently discovered nickelate superconductors3,4,5,6,7,8,9,10, a large antiferromagnetic exchange energy has been reported, which implies the existence of strong electronic correlations11. However, signatures of a broken-symmetry state other than superconductivity have not yet been observed. Here we observe charge ordering in infinite-layer nickelates La1−xSrxNiO2 using resonant X-ray scattering. The parent compound orders along the Ni–O bond direction with an incommensurate wavevector, distinct from the stripe order observed in other nickelates12,13,14 that propagates along a direction 45° to the Ni–O bond. The resonance profile we measure indicates that ordering originates from the nickelate layers and induces a parasitic charge modulation of lanthanum electrons. Upon doping, the charge order diminishes and its wavevector shifts towards commensurate, hinting that strong electronic correlations are likely to be responsible for the ordered state. Our results suggest that the existence of charge order and its potential interplay with antiferromagnetic fluctuations and superconductivity are important themes in nickel-based superconductors.
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Jul 2022
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