I21-Resonant Inelastic X-ray Scattering (RIXS)
|
H.
Lu
,
M.
Rossi
,
A.
Nag
,
M.
Osada
,
D. F.
Li
,
K.
Lee
,
B. Y.
Wang
,
M.
Garcia-Fernandez
,
S.
Agrestini
,
Z. X.
Shen
,
E. M.
Been
,
B.
Moritz
,
T. P.
Devereaux
,
J.
Zaanen
,
H. Y.
Hwang
,
K.-J.
Zhou
,
W.-S.
Lee
Diamond Proposal Number(s):
[25165]
Abstract: The discovery of superconductivity in infinite-layer nickelates brings us tantalizingly close to a material class that mirrors the cuprate superconductors. We measured the magnetic excitations in these nickelates using resonant inelastic x-ray scattering at the Ni L3-edge. Undoped NdNiO2 possesses a branch of dispersive excitations with a bandwidth of approximately 200 milli–electron volts, which is reminiscent of the spin wave of strongly coupled, antiferromagnetically aligned spins on a square lattice. The substantial damping of these modes indicates the importance of coupling to rare-earth itinerant electrons. Upon doping, the spectral weight and energy decrease slightly, whereas the modes become overdamped. Our results highlight the role of Mottness in infinite-layer nickelates.
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Jul 2021
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I21-Resonant Inelastic X-ray Scattering (RIXS)
|
Diamond Proposal Number(s):
[18469]
Open Access
Abstract: Resonant inelastic x-ray scattering (RIXS) is a powerful probe of elementary excitations in solids. It is now widely applied to study magnetic excitations. However, its complex cross section means that RIXS has been more difficult to interpret than inelastic neutron scattering (INS). Here we report
∼
37
meV resolution RIXS measurements of the magnetic excitations in
La
2
CuO
4
, the antiferromagnetic parent of one system of high-temperature superconductors. At high energies (
∼
2
eV), the RIXS spectra show angular-dependent
d
d
orbital excitations in agreement with previous RIXS studies but show new structure. They are interpreted with single-site multiplet calculations. At low energies (
≲
0.3
eV), we model the wave-vector-dependent single magnon RIXS intensity as the product of the calculated single-ion spin-flip RIXS cross section and the dynamical structure factor
S
(
Q
,
ω
)
of the spin-wave excitations. When
S
(
Q
,
ω
)
is extracted from our data, the wave-vector-dependence of the single-magnon pole intensity shows a similar variation to that observed by INS. Our results confirm that suitably corrected RIXS data can yield the genuine wave-vector and energy dependence of
S
(
Q
,
ω
)
for a cuprate antiferromagnet. In addition to spin waves, our data show structured multimagnon excitations with dispersing peaks in the intensity at energies higher than the single-magnon excitations.
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Jun 2021
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I21-Resonant Inelastic X-ray Scattering (RIXS)
|
Haiyu
Lu
,
Matteo
Rossi
,
Jung-Ho
Kim
,
Hasan
Yavas
,
Ayman
Said
,
Abhishek
Nag
,
Mirian
Garcia-Fernandez
,
Stefano
Agrestini
,
Ke-Jin
Zhou
,
Chunjing
Jia
,
Brian
Moritz
,
Thomas P.
Devereaux
,
Zhi-Xun
Shen
,
Wei-Sheng
Lee
Diamond Proposal Number(s):
[25165]
Abstract: We utilized high-energy-resolution resonant inelastic x-ray scattering (RIXS) at both the Ta and Ni
L
3
edges to map out element-specific particle-hole excitations in
Ta
2
Ni
Se
5
across the phase transition. Our results reveal a momentum-dependent gaplike feature in the low-energy spectrum, which agrees well with the band gap in element-specific joint density of states calculations based on ab initio estimates of the electronic structure in both the low-temperature monoclinic and high-temperature orthorhombic structures. Below
T
c
, the RIXS energy-momentum map shows a minimal gap at the Brillouin zone center
(
∼
0.16
eV
)
, confirming that
Ta
2
Ni
Se
5
possesses a direct band gap in its low-temperature ground state. However, inside the gap, no signature of anticipated collective modes with an energy scale comparable to the gap size can be identified. Upon increasing the temperature to above
T
c
, whereas the gap at the zone center closes, the RIXS map at finite momenta still possesses the gross features of the low-temperature map, suggesting a substantial mixing between the Ta and Ni orbits in the conduction and valence bands, which does not change substantially across the phase transition. Our experimental observations and comparison to the theoretical calculations lend further support to the phase transition and the corresponding gap opening in
Ta
2
Ni
Se
5
being largely structural by nature, with a possible minor contribution from the putative exciton condensate.
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Jun 2021
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I21-Resonant Inelastic X-ray Scattering (RIXS)
|
Qisi
Wang
,
Karin
Von Arx
,
Masafumi
Horio
,
Deepak John
Mukkattukavil
,
Julia
Kuespert
,
Yasmine
Sassa
,
Thorsten
Schmitt
,
Abhishek
Nag
,
Sunseng
Pyon
,
Tomohiro
Takayama
,
Hidenori
Takagi
,
Mirian
Garcia-Fernandez
,
Ke-Jin
Zhou
,
Johan
Chang
Diamond Proposal Number(s):
[24481]
Open Access
Abstract: Charge order is universal to all hole-doped cuprates. Yet, the driving interactions remain an unsolved problem. Electron-electron interaction is widely believed to be essential, whereas the role of electron-phonon interaction is unclear. We report an ultrahigh-resolution resonant inelastic x-ray scattering (RIXS) study of the in-plane bond-stretching phonon mode in stripe-ordered cuprate La1.675Eu0.2Sr0.125CuO4. Phonon softening and lifetime shortening are found around the charge ordering wave vector. In addition to these self-energy effects, the electron-phonon coupling is probed by its proportionality to the RIXS cross section. We find an enhancement of the electron-phonon coupling around the charge-stripe ordering wave vector upon cooling into the low-temperature tetragonal structure phase. These results suggest that, in addition to electronic correlations, electron-phonon coupling contributes substantially to the emergence of long-range charge-stripe order in cuprates.
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Jun 2021
|
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I21-Resonant Inelastic X-ray Scattering (RIXS)
|
Jonathan
Pelliciari
,
Seher
Karakuzu
,
Qi
Song
,
Riccardo
Arpaia
,
Abhishek
Nag
,
Matteo
Rossi
,
Jiemin
Li
,
Tianlun
Yu
,
Xiaoyang
Chen
,
Rui
Peng
,
Mirian
Garcia-Fernandez
,
Andrew C.
Walters
,
Qisi
Wang
,
Jun
Zhao
,
Giacomo
Ghiringhelli
,
Donglai
Feng
,
Thomas A.
Maier
,
Ke-Jin
Zhou
,
Steven
Johnston
,
Riccardo
Comin
Diamond Proposal Number(s):
[18883]
Open Access
Abstract: In ultrathin films of FeSe grown on SrTiO3 (FeSe/STO), the superconducting transition temperature Tc is increased by almost an order of magnitude, raising questions on the pairing mechanism. As in other superconductors, antiferromagnetic spin fluctuations have been proposed to mediate SC making it essential to study the evolution of the spin dynamics of FeSe from the bulk to the ultrathin limit. Here, we investigate the spin excitations in bulk and monolayer FeSe/STO using resonant inelastic x-ray scattering (RIXS) and quantum Monte Carlo (QMC) calculations. Despite the absence of long-range magnetic order, bulk FeSe displays dispersive magnetic excitations reminiscent of other Fe-pnictides. Conversely, the spin excitations in FeSe/STO are gapped, dispersionless, and significantly hardened relative to its bulk counterpart. By comparing our RIXS results with simulations of a bilayer Hubbard model, we connect the evolution of the spin excitations to the Fermiology of the two systems revealing a remarkable reconfiguration of spin excitations in FeSe/STO, essential to understand the role of spin fluctuations in the pairing mechanism.
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May 2021
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I21-Resonant Inelastic X-ray Scattering (RIXS)
|
Diamond Proposal Number(s):
[25589]
Open Access
Abstract: Layered Li-rich transition metal oxides undergo O-redox, involving the oxidation of the O2− ions charge compensated by extraction of Li+ ions. Recent results have shown that for 3d transition metal oxides the oxidized O2− forms molecular O2 trapped in the bulk particles. Other forms of oxidised O2− such as O22− or (O–O)n− with long bonds have been proposed, based especially on work on 4 and 5d transition metal oxides, where TM–O bonding is more covalent. Here, we show, using high resolution RIXS that molecular O2 is formed in the bulk particles on O2‒ oxidation in the archetypal Li-rich ruthenates and iridate compounds, Li2RuO3, Li2Ru0.5Sn0.5O3 and Li2Ir0.5Sn0.5O3. The results indicate that O-redox occurs across 3, 4, and 5d transition metal oxides, forming O2, i.e. the greater covalency of the 4d and 5d compounds still favours O2. RIXS and XAS data for Li2IrO3 are consistent with a charge compensation mechanism associated primarily with Ir redox up to and beyond the 5+ oxidation state, with no evidence of O–O dimerization.
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May 2021
|
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I21-Resonant Inelastic X-ray Scattering (RIXS)
|
J.
Li
,
L.
Xu
,
M.
Garcia-Fernandez
,
A.
Nag
,
H. C.
Robarts
,
A. C.
Walters
,
X.
Liu
,
J.
Zhou
,
K.
Wohlfeld
,
J.
Van Den Brink
,
H.
Ding
,
K.-J.
Zhou
Open Access
Abstract: We explore the existence of the collective orbital excitations, orbitons, in the canonical orbital system
KCuF
3
using the Cu
L
3
-edge resonant inelastic x-ray scattering. We show that the nondispersive high-energy peaks result from the
Cu
2
+
d
d
orbital excitations. These high-energy modes display good agreement with the ab initio quantum chemistry calculation, indicating that the
d
d
excitations are highly localized. At the same time, the low-energy excitations present clear dispersion. They match extremely well with the two-spinon continuum following the comparison with Müller ansatz calculations. The localized
d
d
excitations and the observation of the strongly dispersive magnetic excitations suggest that the orbiton dispersion is below the resolution detection limit. Our results can reconcile with the strong local Jahn-Teller effect in
KCuF
3
, which predominantly drives orbital ordering.
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Mar 2021
|
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I21-Resonant Inelastic X-ray Scattering (RIXS)
|
J. Q.
Lin
,
P.
Villar Arribi
,
G.
Fabbris
,
A. s.
Botana
,
D.
Meyers
,
H.
Miao
,
Y.
Shen
,
D. G.
Mazzone
,
J.
Feng
,
G. S.
Chiuzbaian
,
A.
Nag
,
A. C.
Walters
,
M.
Garcia-Fernandez
,
K.-J.
Zhou
,
J.
Pelliciari
,
I.
Jarrige
,
J. W.
Freeland
,
J.
Zhang
,
J. F.
Mitchell
,
V.
Bisogni
,
X.
Liu
,
M. R.
Norman
,
M. P. M.
Dean
Diamond Proposal Number(s):
[18519]
Abstract: The discovery of superconductivity in a
d
9
−
δ
nickelate has inspired disparate theoretical perspectives regarding the essential physics of this class of materials. A key issue is the magnitude of the magnetic superexchange, which relates to whether cuprate-like high-temperature nickelate superconductivity could be realized. We address this question using Ni
L
-edge and O
K
-edge spectroscopy of the reduced
d
9
−
1
/
3
trilayer nickelates
R
4
Ni
3
O
8
(where
R
=
La
, Pr) and associated theoretical modeling. A magnon energy scale of
∼
80
meV
resulting from a nearest-neighbor magnetic exchange of
J
=
69
(
4
)
meV
is observed, proving that
d
9
−
δ
nickelates can host a large superexchange. This value, along with that of the Ni-O hybridization estimated from our O
K
-edge data, implies that trilayer nickelates represent an intermediate case between the infinite-layer nickelates and the cuprates. Layered nickelates thus provide a route to testing the relevance of superexchange to nickelate superconductivity.
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Feb 2021
|
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I21-Resonant Inelastic X-ray Scattering (RIXS)
|
A.
Nag
,
M.
Zhu
,
M.
Bejas
,
J.
Li
,
H. C.
Robarts
,
H.
Yamase
,
A. N.
Petsch
,
D.
Song
,
H.
Eisaki
,
A. C.
Walters
,
M.
Garcia-Fernandez
,
A.
Greco
,
S. M.
Hayden
,
K.
Zhou
Diamond Proposal Number(s):
[24587]
Open Access
Abstract: High
T
c
superconductors show a rich variety of phases associated with their charge degrees of freedom. Valence charges can give rise to charge ordering or acoustic plasmons in these layered cuprate superconductors. While charge ordering has been observed for both hole- and electron-doped cuprates, acoustic plasmons have only been found in electron-doped materials. Here, we use resonant inelastic x-ray scattering to observe the presence of acoustic plasmons in two families of hole-doped cuprate superconductors (
La
1.84
Sr
0.16
CuO
4
and
Bi
2
Sr
1.6
La
0.4
CuO
6
+
δ
), crucially completing the picture. Interestingly, in contrast to the quasistatic charge ordering which manifests at both Cu and O sites, the observed acoustic plasmons are predominantly associated with the O sites, revealing a unique dichotomy in the behavior of valence charges in hole-doped cuprates.
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Dec 2020
|
|
B18-Core EXAFS
I21-Resonant Inelastic X-ray Scattering (RIXS)
|
Diamond Proposal Number(s):
[20363, 23889]
Open Access
Abstract: In the search for high energy density cathodes for next-generation lithium-ion batteries, the disordered rocksalt oxyfluorides are receiving significant attention due to their high capacity and lower voltage hysteresis compared with ordered Li-rich layered compounds. However, a deep understanding of these phenomena and their redox chemistry remains incomplete. Using the archetypal oxyfluoride, Li2MnO2F, we show that the oxygen redox process in such materials involves the formation of molecular O2 trapped in the bulk structure of the charged cathode, which is reduced on discharge. The molecular O2 is trapped rigidly within vacancy clusters and exhibits minimal mobility unlike free gaseous O2, making it more characteristic of a solid-like environment. The Mn redox process occurs between octahedral Mn3+ and Mn4+ with no evidence of tetrahedral Mn5+ or Mn7+. We furthermore derive the relationship between local coordination environment and redox potential; this gives rise to the observed overlap in Mn and O redox couples and reveals that the onset potential of oxide ion oxidation is determined by the degree of ionicity around oxygen, which extends models based on linear Li–O–Li configurations. This study advances our fundamental understanding of redox mechanisms in disordered rocksalt oxyfluorides, highlighting their promise as high capacity cathodes.
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Dec 2020
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