I21-Resonant Inelastic X-ray Scattering (RIXS)
|
Jiemin
Li
,
Abhishek
Nag
,
Jonathan
Pelliciari
,
Hannah
Robarts
,
Andrew
Walters
,
Mirian
Garcia-fernandez
,
Hiroshi
Eisaki
,
Dongjoon
Song
,
Hong
Ding
,
Steven
Johnston
,
Riccardo
Comin
,
Kejin
Zhou
Diamond Proposal Number(s):
[19886, 21184, 21277]
Open Access
Abstract: Charge-density waves (CDWs) are ubiquitous in underdoped cuprate superconductors. As a modulation of the valence electron density, CDWs in hole-doped cuprates possess both Cu-3d and O-2p orbital character owing to the strong hybridization of these orbitals near the Fermi level. Here, we investigate underdoped Bi2Sr1.4La0.6CuO6+δ using resonant inelastic X-ray scattering (RIXS) and find that a short-range CDW exists at both Cu and O sublattices in the copper-oxide (CuO2) planes with a comparable periodicity and correlation length. Furthermore, we uncover bond-stretching and bond-buckling phonon anomalies concomitant to the CDWs. Comparing to slightly overdoped Bi2Sr1.8La0.2CuO6+δ, where neither CDWs nor phonon anomalies appear, we highlight that a sharp intensity anomaly is induced in the proximity of the CDW wavevector (QCDW) for the bond-buckling phonon, in concert with the diffused intensity enhancement of the bond-stretching phonon at wavevectors much greater than QCDW. Our results provide a comprehensive picture of the quasistatic CDWs, their dispersive excitations, and associated electron-phonon anomalies, which are key for understanding the competing electronic instabilities in cuprates.
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Jun 2020
|
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I21-Resonant Inelastic X-ray Scattering (RIXS)
|
J. Q.
Lin
,
H.
Miao
,
D. G.
Mazzone
,
G. D.
Gu
,
A.
Nag
,
A. C.
Walters
,
M.
Garcia-fernandez
,
A.
Barbour
,
J.
Pelliciari
,
I.
Jarrige
,
M.
Oda
,
K.
Kurosawa
,
N.
Momono
,
K.
Zhou
,
V.
Bisogni
,
X.
Liu
,
M. P. M.
Dean
Diamond Proposal Number(s):
[22261]
Abstract: The discovery of charge-density-wave-related effects in the resonant inelastic x-ray scattering spectra of cuprates holds the tantalizing promise of clarifying the interactions that stabilize the electronic order. Here, we report a comprehensive resonant inelastic x-ray scattering study of
La
2
−
x
Sr
x
CuO
4
finding that charge-density wave effects persist up to a remarkably high doping level of
x
=
0.21
before disappearing at
x
=
0.25
. The inelastic excitation spectra remain essentially unchanged with doping despite crossing a topological transition in the Fermi surface. This indicates that the spectra contain little or no direct coupling to electronic excitations near the Fermi surface, rather they are dominated by the resonant cross section for phonons and charge-density-wave-induced phonon softening. We interpret our results in terms of a charge-density wave that is generated by strong correlations and a phonon response that is driven by the charge-density-wave-induced modification of the lattice.
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May 2020
|
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I21-Resonant Inelastic X-ray Scattering (RIXS)
|
Q.
Wang
,
M.
Horio
,
K.
Von Arx
,
Y.
Shen
,
D.
John Mukkattukavil
,
Y.
Sassa
,
O.
Ivashko
,
C. E.
Matt
,
S.
Pyon
,
T.
Takayama
,
H.
Takagi
,
T.
Kurosawa
,
N.
Momono
,
M.
Oda
,
T.
Adachi
,
S. M.
Haidar
,
Y.
Koike
,
Y.
Tseng
,
W.
Zhang
,
J.
Zhao
,
K.
Kummer
,
M.
Garcia-fernandez
,
K.
Zhou
,
N. B.
Christensen
,
H. M.
Ronnow
,
T.
Schmitt
,
J.
Chang
Diamond Proposal Number(s):
[20828, 24481]
Abstract: We use resonant inelastic x-ray scattering to investigate charge-stripe correlations in
La
1.675
Eu
0.2
Sr
0.125
CuO
4
. By differentiating elastic from inelastic scattering, it is demonstrated that charge-stripe correlations precede both the structural low-temperature tetragonal phase and the transport-defined pseudogap onset. The scattering peak amplitude from charge stripes decays approximately as
T
−
2
towards our detection limit. The in-plane integrated intensity, however, remains roughly temperature independent. Therefore, although the incommensurability shows a remarkably large increase at high temperature, our results are interpreted via a single scattering constituent. In fact, direct comparison to other stripe-ordered compounds (
La
1.875
Ba
0.125
CuO
4
,
La
1.475
Nd
0.4
Sr
0.125
CuO
4
, and
La
1.875
Sr
0.125
CuO
4
) suggests a roughly constant integrated scattering intensity across all these compounds. Our results therefore provide a unifying picture for the charge-stripe ordering in La-based cuprates. As charge correlations in
La
1.675
Eu
0.2
Sr
0.125
CuO
4
extend beyond the low-temperature tetragonal and pseudogap phase, their emergence heralds a spontaneous symmetry breaking in this compound.
|
May 2020
|
|
I21-Resonant Inelastic X-ray Scattering (RIXS)
|
A.
Nag
,
H. C.
Robarts
,
F.
Wenzel
,
J.
Li
,
H.
Elnaggar
,
R.-p.
Wang
,
A.
Walters
,
M.
Garcia-fernandez
,
F. M. F.
De Groot
,
M. W.
Haverkort
,
K.
Zhou
Open Access
Abstract: Understanding many-body physics of elementary excitations has advanced our control over material properties. Here, we study spin-flip excitations in NiO using Ni
L3-edge resonant inelastic x-ray scattering (RIXS) and present a strikingly different resonant energy behavior between single and double spin-flip excitations. Comparing our results with single-site full-multiplet ligand field theory calculations we find that the spectral weight of the double-magnon excitations originates primarily from the double spin-flip transition of the quadrupolar RIXS process within a single magnetic site. Quadrupolar spin-flip processes are among the least studied excitations, despite being important for multiferroic or spin-nematic materials due to their difficult detection. We identify intermediate state multiplets and intra-atomic core-valence exchange interactions as the key many-body factors determining the fate of such excitations. RIXS resonant energy dependence can act as a convincing proof of existence of nondipolar higher-ranked magnetic orders in systems for which, only theoretical predictions are available.
|
Feb 2020
|
|
I21-Resonant Inelastic X-ray Scattering (RIXS)
|
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
Diamond Proposal Number(s):
[22009]
Abstract: The search continues for nickel oxide-based materials with electronic properties similar to cuprate high-temperature superconductors. The recent discovery of superconductivity in the doped infinite-layer nickelate NdNiO2 has strengthened these efforts. Here, we use X-ray spectroscopy and density functional theory to show that the electronic structure of LaNiO2 and NdNiO2, while similar to the cuprates, includes significant distinctions. Unlike cuprates, the rare-earth spacer layer in the infinite-layer nickelate supports a weakly interacting three-dimensional 5d metallic state, which hybridizes with a quasi-two-dimensional, strongly correlated state with
3
d
x
2
−
y
2
3dx2−y2
symmetry in the NiO2 layers. Thus, the infinite-layer nickelate can be regarded as a sibling of the rare-earth intermetallics, which are well known for heavy fermion behaviour, where the NiO2 correlated layers play an analogous role to the 4f states in rare-earth heavy fermion compounds. This Kondo- or Anderson-lattice-like ‘oxide-intermetallic’ replaces the Mott insulator as the reference state from which superconductivity emerges upon doping.
|
Jan 2020
|
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I21-Resonant Inelastic X-ray Scattering (RIXS)
|
Jiaqi
Lin
,
Jie
Yuan
,
Kui
Jin
,
Zhiping
Yin
,
Gang
Li
,
Kejin
Zhou
,
Xingye
Lu
,
Marcus
Dantz
,
Thorsten
Schmitt
,
Hong
Ding
,
Haizhong
Guo
,
Mark P. M.
Dean
,
Xuerong
Liu
Open Access
Abstract: Electron correlations play a dominant role in the charge dynamics of the cuprates. We use resonant inelastic X-ray scattering (RIXS) to track the doping dependence of the collective charge excitations in electron doped La
2−x
2−x
Ce
x
x
CuO
4
4
(LCCO). From the resonant energy dependence and the out-of-plane momentum dependence, the charge excitations are identified as three-dimensional (3D) plasmons, which reflect the nature of the electronic structure and Coulomb repulsion on both short and long lengthscales. With increasing electron doping, the plasmon excitations increase monotonically in energy, a consequence of the electron correlation effect on electron structure near the Fermi surface (FS). Importantly, the plasmon excitations evolve from a broad feature into a well-defined peak with much increased life time, revealing the evolution of the electrons from incoherent states to coherent quasi-particles near the FS. Such evolution marks the reduction of the short-range electronic correlation, and thus the softening of the Mottness of the system with increasing electron doping.
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Jan 2020
|
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I21-Resonant Inelastic X-ray Scattering (RIXS)
|
Robert A.
House
,
Urmimala
Maitra
,
Miguel A.
Pérez-osorio
,
Juan G.
Lozano
,
Liyu
Jin
,
James W.
Somerville
,
Laurent C.
Duda
,
Abhishek
Nag
,
Andrew
Walters
,
Kejin
Zhou
,
Matthew R.
Roberts
,
Peter G.
Bruce
Abstract: Alkali-rich transition metal oxide intercalation cathodes can increase the energy density of Li and Na-ion batteries by storing charge on the oxide and transition metal (TM) ions1–10. The high voltage associated with oxidation of O2- on the first charge is not recovered on discharge, resulting in significantly reduced energy density11. Displacement of TM ions from the TM to alkali metal layers has been proposed to explain the first cycle voltage loss9,12–16. By comparing two closely related intercalation cathodes, Na0.75[Li0.25Mn0.75]O2 and Na0.6[Li0.2Mn0.8]O2, we show that the first cycle voltage hysteresis is determined by the superstructure, specifically the local ordering of Li/TM ions in the TM layers. The honeycomb superstructure of Na0.75[Li0.25Mn0.75]O2, present in almost all O-redox compounds, is lost on charging, driven, in part, by formation of molecular O2 inside the solid. The O2 molecules are cleaved on discharge reforming O2-, but the Mn ions have migrated in the plane changing the coordination around O2- significantly lowering the voltage on discharge (hysteresis). The ribbon superstructure in Na0.6[Li0.2Mn0.8]O2 inhibits Mn disorder and hence O2 formation, suppressing hysteresis and promoting stable electron holes on O2- which are revealed by XAS. The results show that voltage hysteresis can be avoided in O-redox cathodes by forming materials with a superstructure (cation ordering) in the TM layers that suppresses TM migration.
|
Dec 2019
|
|
I21-Resonant Inelastic X-ray Scattering (RIXS)
|
Diamond Proposal Number(s):
[18469, 18512]
Abstract: We report high-resolution resonant inelastic x-ray scattering (RIXS) measurements of the collective spin fluctuations in three compositions of the superconducting cuprate system
La
2
−
x
Sr
x
CuO
4
. We have mapped out the excitations throughout much of the two-dimensional
(
h
,
k
)
Brillouin zone. The spin fluctuations in
La
2
−
x
Sr
x
CuO
4
are found to be fairly well described by a damped harmonic oscillator model, thus our data allows us to determine the full wave vector dependence of the damping parameter. This parameter increases with doping and is largest along the
(
h
,
h
) line, where it is peaked near
(
0.2
,
0.2
)
. We have used a new procedure to determine the absolute wave vector dependent susceptibility for the doped compositions
La
2
−
x
Sr
x
CuO
4
(
x
=
0.12
,
0.16
)
by normalizing our data to
La
2
CuO
4
measurements made with inelastic neutron scattering (INS). We find that the evolution with doping of the intensity of high-energy excitations measured by RIXS and INS is consistent. For the doped compositions, the wave vector dependent susceptibility is much larger at
(
1
4
,
1
4
)
than at
(
1
2
,
0
)
. It increases rapidly along the
(
h
,
h
)
line towards the antiferromagnetic wave vector of the parent compound
(
1
2
,
1
2
)
. Thus, the strongest magnetic excitations, and those predicted to favor superconductive pairing, occur towards the
(
1
2
,
1
2
)
position as observed by INS.
|
Dec 2019
|
|
I21-Resonant Inelastic X-ray Scattering (RIXS)
|
J. G.
Vale
,
C. D.
Dashwood
,
E.
Paris
,
L. S. I.
Veiga
,
Mirian
Garcia-fernandez
,
A.
Nag
,
A.
Walters
,
K.
Zhou
,
I.-m.
Pietsch
,
Anton
Jesche
,
P.
Gegenwart
,
R.
Coldea
,
T.
Schmitt
,
D. F.
Mcmorrow
Diamond Proposal Number(s):
[20569]
Abstract: The excitations in honeycomb
α
−
Li
2
IrO
3
have been investigated with high-resolution resonant inelastic x-ray scattering (RIXS) at the O
K
edge. The low-energy response is dominated by a fully resolved ladder of excitations, which we interpret as being due to multiphonon processes in the presence of strong electron-phonon coupling (EPC). At higher energies, the orbital excitations are shown to be dressed by phonons. The high quality of the data permits a quantitative test of the analytical model for the RIXS cross section, which has been proposed to describe EPC in transition-metal oxides (TMOs). We find that the magnitude of the EPC is comparable to that found for a range of
3
d
TMOs. This indicates that EPC may be of equal importance in determining the phenomenology displayed by corresponding
5
d
-based systems.
|
Dec 2019
|
|
|
|
J.
Schlappa
,
U.
Kumar
,
K. J.
Zhou
,
S.
Singh
,
M.
Mourigal
,
V. N.
Strocov
,
A.
Revcolevschi
,
L.
Patthey
,
H. M.
Ronnow
,
S.
Johnston
,
T.
Schmitt
Open Access
Abstract: One-dimensional (1D) magnetic insulators have attracted significant interest as a platform for studying quasiparticle fractionalization, quantum criticality, and emergent phenomena. The spin-1/2 Heisenberg chain with antiferromagnetic nearest neighbour interactions is an important reference system; its elementary magnetic excitations are spin-1/2 quasiparticles called spinons that are created in even numbers. However, while the excitation continuum associated with two-spinon states is routinely observed, the study of four-spinon and higher multi-spinon states is an open area of research. Here we show that four-spinon excitations can be accessed directly in Sr2CuO3 using resonant inelastic x-ray scattering (RIXS) in a region of phase space clearly separated from the two-spinon continuum. Our finding is made possible by the fundamental differences in the correlation function probed by RIXS in comparison to other probes. This advance holds promise as a tool in the search for novel quantum states and quantum spin liquids.
|
Dec 2018
|
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