I21-Resonant Inelastic X-ray Scattering (RIXS)
|
Marli R.
Cantarino
,
Rafael M. P.
Teixeira
,
Kevin R.
Pakuszewski
,
Wagner R.
Da Silva Neto
,
Juliana G.
De Abrantes
,
Mirian
Garcia-Fernandez
,
Pascoal G.
Pagliuso
,
Cris
Adriano
,
Claude
Monney
,
Thorsten
Schmitt
,
Eric C.
Andrade
,
Fernando A.
Garcia
Diamond Proposal Number(s):
[33194]
Open Access
Abstract: In doped Hund's metals, such as the iron-based superconductors, effects like charge doping and chemical pressure are often considered the dominant factors. Partial chemical substitution, however, inevitably introduces disorder. Here, we investigate spin excitations in Ba(Fe1−𝑥Cr𝑥)2As2 (CrBFA) by high-resolution resonant inelastic x-ray scattering for samples with 𝑥=0,0.035, and 0.085. In CrBFA, Cr acts as a hole dopant, but also introduces localized spins that compete with Fe-derived magnetic excitations. We found that the Fe-derived magnetic excitations are softened and damped, becoming overdamped for 𝑥=0.085. At this doping level, complementary angle-resolved photoemission spectroscopy measurements show increased electronic localization and a suppression of the nematic 𝑑𝑥𝑧/𝑑𝑦𝑧 band splitting present in the parent compound. We thus propose a localized spin model that explicitly incorporates substitutional disorder and Cr local moments, successfully reproducing our key observations. Our findings reveal a case where disorder dominates over charge doping in the case of a Hund's metal.
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Feb 2026
|
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I21-Resonant Inelastic X-ray Scattering (RIXS)
|
Teguh Citra
Asmara
,
Robert J.
Green
,
Andreas
Suter
,
Yuan
Wei
,
Wenliang
Zhang
,
Daniel
Knez
,
Grant
Harris
,
Yi
Tseng
,
Tianlun
Yu
,
Davide
Betto
,
Mirian
Garcia-Fernandez
,
Stefano
Agrestini
,
Yannick Maximilian
Klein
,
Neeraj
Kumar
,
Carlos W.
Galdino
,
Zaher
Salman
,
Thomas
Prokscha
,
Marisa
Medarde
,
Elisabeth
Müller
,
Yona
Soh
,
Nicholas B.
Brookes
,
Ke-Jin
Zhou
,
Milan
Radovic
,
Thorsten
Schmitt
Diamond Proposal Number(s):
[28665]
Open Access
Abstract: Strongly-correlated transition-metal oxides are widely known for their various exotic phenomena. This is exemplified by rare-earth nickelates such as LaNiO3, which possess intimate interconnections between their electronic, spin, and lattice degrees of freedom. Their properties can be further enhanced by pairing them in hybrid heterostructures, which can lead to hidden phases and emergent phenomena. An important example is the LaNiO3/LaTiO3 superlattice, where an interlayer electron transfer has been observed from LaTiO3 into LaNiO3 leading to a high-spin state. However, macroscopic emergence of magnetic order associated with this high-spin state has so far not been observed. Here, by using muon spin rotation, x-ray absorption, and resonant inelastic x-ray scattering, direct evidence of an emergent antiferromagnetic order with high magnon energy and exchange interactions at the LaNiO3/LaTiO3 interface is presented. As the magnetism is purely interfacial, a single LaNiO3/LaTiO3 interface can essentially behave as an atomically thin strongly-correlated quasi-2D antiferromagnet, potentially allowing its technological utilization in advanced spintronic devices. Furthermore, its strong quasi-2D magnetic correlations, orbitally-polarized planar ligand holes, and layered superlattice design make its electronic, magnetic, and lattice configurations resemble the precursor states of superconducting cuprates and nickelates, but with an S→1 spin state instead.
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Aug 2024
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I21-Resonant Inelastic X-ray Scattering (RIXS)
|
Leonardo
Martinelli
,
Krzysztof
Wohlfeld
,
Jonathan
Pelliciari
,
Riccardo
Arpaia
,
Nicholas B.
Brookes
,
Daniele
Di Castro
,
Mirian
Garcia-Fernandez
,
Mingu
Kang
,
Yoshiharu
Krockenberger
,
Kurt
Kummer
,
Daniel E.
Mcnally
,
Eugenio
Paris
,
Thorsten
Schmitt
,
Hideki
Yamamoto
,
Andrew
Walters
,
Ke-Jin
Zhou
,
Lucio
Braicovich
,
Riccardo
Comin
,
Marco
Moretti Sala
,
Thomas P.
Devereaux
,
Maria
Daghofer
,
Giacomo
Ghiringhelli
Diamond Proposal Number(s):
[20690]
Abstract: We have investigated the
3
d
orbital excitations in
CaCuO
2
(CCO),
Nd
2
CuO
4
(NCO), and
La
2
CuO
4
(LCO) using high-resolution resonant inelastic x-ray scattering. In LCO they behave as well-localized excitations, similarly to several other cuprates. On the contrary, in CCO and NCO the
d
x
y
orbital clearly disperses, pointing to a collective character of this excitation (orbiton) in compounds without apical oxygen. We ascribe the origin of the dispersion as stemming from a substantial next-nearest-neighbor (NNN) orbital superexchange. Such an exchange leads to the liberation of the orbiton from its coupling to magnons, which is associated with the orbiton hopping between nearest neighbor copper sites. Finally, we show that the exceptionally large NNN orbital superexchange can be traced back to the absence of apical oxygens suppressing the charge transfer energy.
|
Feb 2024
|
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I21-Resonant Inelastic X-ray Scattering (RIXS)
|
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.
|
Aug 2022
|
|
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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I05-ARPES
|
Niels B. M.
Schroeter
,
Iñigo
Robredo
,
Sebastian
Klemenz
,
Robert J.
Kirby
,
Jonas A.
Krieger
,
Ding
Pei
,
Tianlun
Yu
,
Samuel
Stolz
,
Thorsten
Schmitt
,
Pavel
Dudin
,
Timur K.
Kim
,
Cephise
Cacho
,
Andreas
Schnyder
,
Aitor
Bergara
,
Vladimir N.
Strocov
,
Fernando
De Juan
,
Maia G.
Vergniory
,
Leslie M.
Schoop
Diamond Proposal Number(s):
[26098, 20617]
Open Access
Abstract: Magnetic Weyl semimetals are a newly discovered class of topological materials that may serve as a platform for exotic phenomena, such as axion insulators or the quantum anomalous Hall effect. Here, we use angle-resolved photoelectron spectroscopy and ab initio calculations to discover Weyl cones in CoS2, a ferromagnet with pyrite structure that has been long studied as a candidate for half-metallicity, which makes it an attractive material for spintronic devices. We directly observe the topological Fermi arc surface states that link the Weyl nodes, which will influence the performance of CoS2 as a spin injector by modifying its spin polarization at interfaces. In addition, we directly observe a minority-spin bulk electron pocket in the corner of the Brillouin zone, which proves that CoS2 cannot be a true half-metal.
|
Dec 2020
|
|
I05-ARPES
|
Niels B. M.
Schroeter
,
Samuel
Stolz
,
Kaustuv
Manna
,
Fernando
De Juan
,
Maia G.
Vergniory
,
Jonas A.
Krieger
,
Ding
Pei
,
Thorsten
Schmitt
,
Pavel
Dudin
,
Timur K.
Kim
,
Cephise
Cacho
,
Barry
Bradlyn
,
Horst
Borrmann
,
Marcus
Schmidt
,
Roland
Widmer
,
Vladimir N.
Strocov
,
Claudia
Felser
Diamond Proposal Number(s):
[24703, 20617]
Open Access
Abstract: Topological semimetals feature protected nodal band degeneracies characterized by a topological invariant known as the Chern number (C). Nodal band crossings with linear dispersion are expected to have at most |C|=4
|
C
|
=
4
, which sets an upper limit to the magnitude of many topological phenomena in these materials. Here, we show that the chiral crystal palladium gallium (PdGa) displays multifold band crossings, which are connected by exactly four surface Fermi arcs, thus proving that they carry the maximal Chern number magnitude of 4. By comparing two enantiomers, we observe a reversal of their Fermi-arc velocities, which demonstrates that the handedness of chiral crystals can be used to control the sign of their Chern numbers.
|
Jul 2020
|
|
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)
|
Jiaqi
Lin
,
Jie
Yuan
,
Kui
Jin
,
Zhiping
Yin
,
Gang
Li
,
Ke-Jin
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.
|
Jan 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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