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.
|
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.
|
May 2021
|
|
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.
|
Mar 2021
|
|
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.
|
Feb 2021
|
|
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.
|
Dec 2020
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I21-Resonant Inelastic X-ray Scattering (RIXS)
|
Roberto
Fumagalli
,
Abhishek
Nag
,
Stefano
Agrestini
,
Mirian
Garcia-Fernandez
,
Andrew C.
Walters
,
Davide
Betto
,
Nicholas B.
Brookes
,
Lucio
Braicovich
,
Ke-Jin
Zhou
,
Giacomo
Ghiringhelli
,
Marco Moretti
Sala
Diamond Proposal Number(s):
[23423]
Abstract: Motivated by the recent synthesis of Ba
CuO
(BCO), a high temperature superconducting cuprate with putative
ground state symmetry, we investigated its electronic structure by means of Cu
x-ray absorption (XAS) and resonant inelastic x-ray scattering (RIXS) at the Cu
edge on a polycrystalline sample. We show that the XAS profile of BCO is characterised by two peaks associated to inequivalent Cu sites, and that its RIXS response features a single, sharp peak associated to crystal-field excitations. We argue that these observations are only partially compatible with the previously proposed crystal structure of BCO. Based on our spectroscopic results and on previously published powder diffraction measurements, we propose a crystalline structure characterized by two inequivalent Cu sites located at alternated planes along the
axis: nominally trivalent Cu(1) belonging to very short Cu-O chains, and divalent Cu(2) in the oxygen deficient CuO
planes. We also analyze the low-energy region of the RIXS spectra to estimate the magnitude of the magnetic interactions in BCO and find that in-plane nearest neighbor superexchange exceeds 120 meV, similarly to that of other layered cuprates. Although these results do not support the pure
ground state scenario, they hint at a significant departure from the common quasi-2D electronic structure of superconducting cuprates of pure
symmetry.
|
Dec 2020
|
|
I21-Resonant Inelastic X-ray Scattering (RIXS)
|
Diamond Proposal Number(s):
[24583]
Open Access
Abstract: Resonant inelastic x-ray spectroscopy at the uranium $N_{4}$ absorption edge at 778 eV has been used to reveal the excitations in UO$_{2}$ up to 1 eV. The earlier (1989) studies by neutron inelastic scattering of the crystal-field states within the $^{3}H_{4}$ multiplet are confirmed. In addition, the first excited state of the $^{3}F_{2}$ multiplet at $\sim$520 meV has been established, and there is a weak signal corresponding to the next excited state at $\sim$920 meV. This represents a successful application of soft x-ray spectroscopy to an actinide sample, and resolves an open question in UO$_{2}$ that has been discussed for 50 years. The technique is described and important caveats are drawn about possible future applications.
|
Oct 2020
|
|
I21-Resonant Inelastic X-ray Scattering (RIXS)
|
W. S.
Lee
,
K.
Zhou
,
M.
Hepting
,
J.
Li
,
A.
Nag
,
A. C.
Walters
,
M.
Garcia-Fernandez
,
H. C.
Robarts
,
M.
Hashimoto
,
H.
Lu
,
B.
Nosarzewski
,
D.
Song
,
H.
Eisaki
,
Z. X.
Shen
,
B.
Moritz
,
J.
Zaanen
,
T. P.
Devereaux
Diamond Proposal Number(s):
[18462]
Abstract: Copper oxide high-TC superconductors possess a number of exotic orders that coexist with or are proximal to superconductivity. Quantum fluctuations associated with these orders may account for the unusual characteristics of the normal state, and possibly affect the superconductivity. Yet, spectroscopic evidence for such quantum fluctuations remains elusive. Here, we use resonant inelastic X-ray scattering to reveal spectroscopic evidence of fluctuations associated with a charge order in nearly optimally doped Bi2Sr2CaCu2O8+δ. In the superconducting state, while the quasielastic charge order signal decreases with temperature, the interplay between charge order fluctuations and bond-stretching phonons in the form of a Fano-like interference increases, an observation that is incompatible with expectations for competing orders. Invoking general principles, we argue that this behaviour reflects the properties of a dissipative system near an order–disorder quantum critical point, where the dissipation varies with the opening of the pseudogap and superconducting gap at low temperatures, leading to the proliferation of quantum critical fluctuations, which melt charge order.
|
Aug 2020
|
|
I21-Resonant Inelastic X-ray Scattering (RIXS)
|
Soonmin
Kang
,
Kangwon
Kim
,
Beom Hyun
Kim
,
Jonghyeon
Kim
,
Kyung Ik
Sim
,
Jae-Ung
Lee
,
Sungmin
Lee
,
Kisoo
Park
,
Seokhwan
Yun
,
Taehun
Kim
,
Abhishek
Nag
,
Andrew
Walters
,
Mirian
Garcia-Fernandez
,
Jiemin
Li
,
Laurent
Chapon
,
Ke-Jin
Zhou
,
Young-Woo
Son
,
Jae Hoon
Kim
,
Hyeonsik
Cheong
,
Je-Geun
Park
Diamond Proposal Number(s):
[18503, 18906]
Abstract: An exciton is the bosonic quasiparticle of electron–hole pairs bound by the Coulomb interaction. Bose–Einstein condensation of this exciton state has long been the subject of speculation in various model systems and examples have been found more recently in optical lattices and two-dimensional materials. Unlike these conventional excitons formed from extended Bloch states, excitonic bound states from intrinsically many-body localized states are rare. Here we show that a spin–orbit-entangled exciton state appears below the Néel temperature of 150 kelvin in NiPS3, an antiferromagnetic van der Waals material. It arises intrinsically from the archetypal many-body states of the Zhang–Rice singlet, and reaches a coherent state assisted by the antiferromagnetic order. Using configuration-interaction theory, we determine the origin of the coherent excitonic excitation to be a transition from a Zhang–Rice triplet to a Zhang–Rice singlet. We combine three spectroscopic tools—resonant inelastic X-ray scattering, photoluminescence and optical absorption—to characterize the exciton and to demonstrate an extremely narrow excitonic linewidth below 50 kelvin. The discovery of the spin–orbit-entangled exciton in antiferromagnetic NiPS3 introduces van der Waals magnets as a platform to study coherent many-body excitons.
|
Jul 2020
|
|
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
,
Ke-Jin
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.
|
Jun 2020
|
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