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
|
|
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.
|
Jun 2021
|
|
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)
|
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
|
|
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)
|
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
|
|
I05-ARPES
|
Niels B. M.
Schröter
,
Ding
Pei
,
Maia G.
Vergniory
,
Yan
Sun
,
Kaustuv
Manna
,
Fernando
De Juan
,
Jonas A.
Krieger
,
Vicky
Süss
,
Marcus
Schmidt
,
Pavel
Dudin
,
Barry
Bradlyn
,
Timur K.
Kim
,
Thorsten
Schmitt
,
Cephise
Cacho
,
Claudia
Felser
,
Vladimir N.
Strocov
,
Yulin
Chen
Diamond Proposal Number(s):
[19883, 21400]
Abstract: Topological semimetals in crystals with a chiral structure (which possess a handedness due to a lack of mirror and inversion symmetries) are expected to display numerous exotic physical phenomena, including fermionic excitations with large topological charge1, long Fermi arc surface states2,3, unusual magnetotransport4 and lattice dynamics5, as well as a quantized response to circularly polarized light6. So far, all experimentally confirmed topological semimetals exist in crystals that contain mirror operations, meaning that these properties do not appear. Here, we show that AlPt is a structurally chiral topological semimetal that hosts new four-fold and six-fold fermions, which can be viewed as a higher spin generalization of Weyl fermions without equivalence in elementary particle physics. These multifold fermions are located at high symmetry points and have Chern numbers larger than those in Weyl semimetals, thus resulting in multiple Fermi arcs that span the full diagonal of the surface Brillouin zone. By imaging these long Fermi arcs, we experimentally determine the magnitude and sign of their Chern number, allowing us to relate their dispersion to the handedness of their host crystal.
|
May 2019
|
|
B18-Core EXAFS
I09-Surface and Interface Structural Analysis
|
Robert A.
House
,
Urmimala
Maitra
,
Liyu
Jin
,
Juan G.
Lozano
,
James W.
Somerville
,
Nicholas H.
Rees
,
Andrew J.
Naylor
,
Laurent C.
Duda
,
Felix
Massel
,
Alan V.
Chadwick
,
Silvia
Ramos
,
David M.
Pickup
,
Daniel E.
Mcnally
,
Xingye
Lu
,
Thorsten
Schmitt
,
Matthew R.
Roberts
,
Peter G.
Bruce
Diamond Proposal Number(s):
[14239, 20870]
Open Access
Abstract: It is possible to increase the charge capacity of transition metal oxide cathodes in alkali-ion batteries by invoking redox reactions on the oxygen. However, oxygen loss often occurs. To explore what affects oxygen loss in oxygen redox materials, we have compared two analogous Na-ion cathodes, P2-Na0.67Mg0.28Mn0.72O2 and P2-Na0.78Li0.25Mn0.75O2. On charging to 4.5 V, >0.4 e- are removed from the oxide ions of these materials, but neither compound exhibits oxygen loss. Li is retained in P2-Na0.78Li0.25Mn0.75O2 but displaced from the transition metal to the alkali metal layers, showing that vacancies in the transition metal layers, which also occur in other oxygen redox compounds that exhibit oxygen loss such as Li[Li0.2Ni0.2Mn0.6]O2, is not a trigger for oxygen loss. On charging at 5 V, P2-Na0.78Li0.25Mn0.75O2 exhibits oxygen loss whereas P2-Na0.67Mg0.28Mn0.72O2 does not. Under these conditions both Na+ and Li+ are removed from P2-Na0.78Li0.25Mn0.75O2 resulting in underbonded oxygen (fewer than 3 cations coordinating oxygen) and surface localised O loss. In contrast, for P2-Na0.67Mg0.28Mn0.72O2, oxygen remains coordinated by at least 2 Mn4+ and 1 Mg2+ ions, stabilising the oxygen and avoiding oxygen loss.
|
Apr 2019
|
|
