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C.
Monney
,
K. J.
Zhou
,
H.
Cercellier
,
Z.
Vydrova
,
M. G.
Garnier
,
G.
Monney
,
V. N.
Strocov
,
H.
Berger
,
H.
Beck
,
T.
Schmitt
,
P.
Aebi
Abstract: In high-resolution resonant inelastic x-ray scattering at the Ti L edge of the charge-density-wave system 1T-TiSe2, we observe sharp low energy loss peaks from electron-hole pair excitations developing at low temperature. These excitations are strongly dispersing as a function of the transferred momentum of light. We show that the unoccupied bands close to the Fermi level can effectively be probed in this broadband material. Furthermore, we extract the order parameter of the charge-density-wave phase from temperature-dependent measurements.
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Jul 2012
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Ke-jin
Zhou
,
Yao-bo
Huang
,
Claude
Monney
,
Xi
Dai
,
Vladimir N.
Strocov
,
Nan-lin
Wang
,
Zhi-guo
Chen
,
Chenglin
Zhang
,
Pengcheng
Dai
,
Luc
Patthey
,
Jeroen
Van Den Brink
,
Hong
Ding
,
Thorsten
Schmitt
Abstract: Motivated by the premise that superconductivity in iron-based superconductors is unconventional and mediated by spin fluctuations, an intense research effort has been focused on characterizing the spin-excitation spectrum in the magnetically ordered parent phases of the Fe pnictides and chalcogenides. For these undoped materials, it is well established that the spin-excitation spectrum consists of sharp, highly dispersive magnons. The fate of these high-energy magnetic modes upon sizable doping with holes is hitherto unresolved. Here we demonstrate, using resonant inelastic X-ray scattering, that optimally hole-doped superconducting Ba0.6K0.4Fe2As2 retains well-defined, dispersive high-energy modes of magnetic origin. These paramagnon modes are softer than, though as intense as, the magnons of undoped antiferromagnetic BaFe2As2. The persistence of spin excitations well into the superconducting phase suggests that the spin fluctuations in Fe-pnictide superconductors originate from a distinctly correlated spin state. This connects Fe pnictides to cuprates, for which, in spite of fundamental electronic structure differences, similar paramagnons are present.
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Feb 2013
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Abstract: Resonant inelastic soft X-ray scattering (RIXS) [1, 2] is a powerful bulk-sensitive photon-in / photonout
spectroscopic and scattering probe of the electronic structure of condensed matter with elemental
sensitivity. It is a unique tool for studying low energy excitations in complex correlated systems, being
sensitive to charge-, orbital-, spin-, and lattice-degrees of freedom [3-7]. Dedicated instrumentation
for soft X-ray RIXS with ultra-high resolution in energy and momentum spaces has become available
thereby enabling characterization of collective excitations such as magnons and phonons. In this presentation
I will give a brief introduction of the I21-RIXS beamline which is currently under construction at
Diamond Light Source in the UK. Details of the key beamline performance, the optical design and the
mechanical designs are to be presented.
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Nov 2015
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Nikolay A.
Bogdanov
,
Valentina
Bisogni
,
Roberto
Kraus
,
Claude
Monney
,
Ke-jin
Zhou
,
Thorsten
Schmitt
,
Jochen
Geck
,
Alexander O
Mitrushchenkov
,
Hermann
Stoll
,
Jeroen
Van Den Brink
,
Liviu
Hozoi
Abstract: In existing theoretical approaches to core-level excitations of transition-metal ions in solids relaxation and polarization effects due to the inner core hole are often ignored or described phenomenologically. Here we set up an ab initio computational scheme that explicitly accounts for such physics in the calculation of x-ray absorption and resonant inelastic x-ray scattering spectra. Good agreement is found with experimental transition-metal L-edge data for the strongly correlated d 9 cuprate Li2CuO2, for which we determine the absolute scattering intensities. The newly developed methodology opens the way for the investigation of even more complex d n electronic structures of group VI B to VIII B correlated oxide compounds.
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Jan 2017
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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.
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Dec 2018
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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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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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I21-Resonant Inelastic X-ray Scattering (RIXS)
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Robert A.
House
,
Urmimala
Maitra
,
Miguel A.
Pérez-osorio
,
Juan G.
Lozano
,
Liyu
Jin
,
James W.
Somerville
,
Laurent C.
Duda
,
Abhishek
Nag
,
Andrew
Walters
,
Ke-jin
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.
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Dec 2019
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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.
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Jan 2020
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|
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.
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Dec 2019
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