I21-Resonant Inelastic X-ray Scattering (RIXS)
|
S.
Agrestini
,
F.
Borgatti
,
P.
Florio
,
J.
Frassineti
,
D.
Fiore Mosca
,
Q.
Faure
,
B.
Detlefs
,
C. j.
Sahle
,
S.
Francoual
,
J.
Choi
,
Mirian
Garcia-Fernandez
,
K.-J.
Zhou
,
V. f.
Mitrović
,
P. m.
Woodward
,
G.
Ghiringhelli
,
C.
Franchini
,
F.
Boscherini
,
S.
Sanna
,
M.
Moretti Sala
Open Access
Abstract: A supposedly nonmagnetic 5𝑑1 double perovskite oxide is investigated by a combination of spectroscopic and theoretical methods, namely, resonant inelastic x-ray scattering, x-ray absorption spectroscopy, magnetic circular dichroism, and multiplet ligand-field calculations. We found that the large spin-orbit coupling admixes the 5𝑑 𝑡2𝑔 and 𝑒𝑔 orbitals, covalency raises the 5𝑑 population well above the nominal value, and the local symmetry is lower than 𝑂ℎ. The obtained electronic interactions account for the finite magnetic moment of Os in this compound and, in general, of 5𝑑1 ions. Our results provide direct evidence of elusive Jahn-Teller distortions, hinting at a strong electron-lattice coupling.
|
Aug 2024
|
|
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)
|
Riccardo
Arpaia
,
Leonardo
Martinelli
,
Marco
Moretti Sala
,
Sergio
Caprara
,
Abhishek
Nag
,
Nicholas B.
Brookes
,
Pietro
Camisa
,
Qizhi
Li
,
Qiang
Gao
,
Xingjiang
Zhou
,
Mirian
Garcia-Fernandez
,
Ke-Jin
Zhou
,
Enrico
Schierle
,
Thilo
Bauch
,
Ying Ying
Peng
,
Carlo
Di Castro
,
Marco
Grilli
,
Floriana
Lombardi
,
Lucio
Braicovich
,
Giacomo
Ghiringhelli
Diamond Proposal Number(s):
[23880]
Open Access
Abstract: The universality of the strange metal phase in many quantum materials is often attributed to the presence of a quantum critical point (QCP), a zero-temperature phase transition ruled by quantum fluctuations. In cuprates, where superconductivity hinders direct QCP observation, indirect evidence comes from the identification of fluctuations compatible with the strange metal phase. Here we show that the recently discovered charge density fluctuations (CDF) possess the right properties to be associated to a quantum phase transition. Using resonant x-ray scattering, we studied the CDF in two families of cuprate superconductors across a wide doping range (up to p = 0.22). At p* ≈ 0.19, the putative QCP, the CDF intensity peaks, and the characteristic energy Δ is minimum, marking a wedge-shaped region in the phase diagram indicative of a quantum critical behavior, albeit with anomalies. These findings strengthen the role of charge order in explaining strange metal phenomenology and provide insights into high-temperature superconductivity.
|
Nov 2023
|
|
I21-Resonant Inelastic X-ray Scattering (RIXS)
|
Yingying
Peng
,
Leonardo
Martinelli
,
Qizhi
Li
,
Matteo
Rossi
,
Matteo
Mitrano
,
Riccardo
Arpaia
,
Marco
Moretti Sala
,
Qiang
Gao
,
Xuefei
Guo
,
Gabriella Maria
De Luca
,
Andrew
Walters
,
Abhishek
Nag
,
Andi
Barbour
,
Genda
Gu
,
Jonathan
Pelliciari
,
Nicholas B.
Brookes
,
Peter
Abbamonte
,
Marco
Salluzzo
,
Xingjiang
Zhou
,
Ke-Jin
Zhou
,
Valentina
Bisogni
,
Lucio
Braicovich
,
Steven
Johnston
,
Giacomo
Ghiringhelli
Diamond Proposal Number(s):
[20012]
Abstract: While electron-phonon coupling (EPC) is crucial for Cooper pairing in conventional superconductors, its role in high-
T
c
superconducting cuprates is debated. Using resonant inelastic x-ray scattering at the oxygen
K
edge, we study the EPC in
Bi
2
Sr
2
Ca
Cu
2
O
8
+
δ
(Bi2212) and
Nd
1
+
x
Ba
2
−
x
Cu
3
O
7
−
δ
(NBCO) at different doping levels ranging from heavily underdoped (
p
=
0.07
) to overdoped (
p
=
0.21
). We analyze the data with a localized Lang-Firsov model that allows for the coherent excitations of two phonon modes. While electronic band dispersion effects are non-negligible, we are able to perform a study of the relative values of EPC matrix elements in these cuprate families. In the case of NBCO, the choice of the excitation energy allows us to disentangle modes related to the CuO chains and the
Cu
O
2
planes. Combining the results from the two families, we find the EPC strength decreases with doping at
q
∥
=
(
−
0.25
,
0
)
r.l.u., but has a nonmonotonic trend as a function of doping at smaller momenta. This behavior is attributed to the screening effect of charge carriers. We also find that the phonon intensity is enhanced in the vicinity of the charge-density-wave excitations while the extracted EPC strength appears to be less sensitive to their proximity. By performing a comparative study of two cuprate families, we are able to identify general trends in the EPC for the cuprates and provide experimental input to theories invoking a synergistic role for this interaction in
d
-wave pairing.
|
Mar 2022
|
|
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
|
|
I11-High Resolution Powder Diffraction
|
Henrik
Jacobsen
,
Hai L.
Feng
,
Andrew J.
Princep
,
Marein C.
Rahn
,
Yanfeng
Guo
,
Jie
Chen
,
Yoshitaka
Matsushita
,
Yoshihiro
Tsujimoto
,
Masahiro
Nagao
,
Dmitry
Khalyavin
,
Pascal
Manuel
,
Claire A.
Murray
,
Christian
Donnerer
,
James G.
Vale
,
Marco
Moretti Sala
,
Kazunari
Yamaura
,
Andrew T.
Boothroyd
Diamond Proposal Number(s):
[9839]
Abstract: We report on the structural, magnetic, and electronic properties of two new double-perovskites synthesized under high pressure,
Pb
2
CaOsO
6
and
Pb
2
ZnOsO
6
. Upon cooling below 80 K,
Pb
2
CaOsO
6
simultaneously undergoes a metal-to-insulator transition and develops antiferromagnetic order.
Pb
2
ZnOsO
6
, on the other hand, remains a paramagnetic metal down to 2 K. The key difference between the two compounds lies in their crystal structures. The Os atoms in
Pb
2
ZnOsO
6
are arranged on an approximately face-centered cubic lattice with strong antiferromagnetic nearest-neighbor exchange couplings. The geometrical frustration inherent to this lattice prevents magnetic order from forming down to the lowest temperatures. In contrast, the unit cell of
Pb
2
CaOsO
6
is heavily distorted up to at least 500 K including antiferroelectriclike displacements of the Pb and O atoms despite metallic conductivity above 80 K. This distortion relieves the magnetic frustration, facilitating magnetic order which, in turn, drives the metal-insulator transition. Our results suggest that the phase transition in
Pb
2
CaOsO
6
is spin driven and could be a rare example of a Slater transition.
|
Dec 2020
|
|
|
|
J. g.
Vale
,
S.
Calder
,
C.
Donnerer
,
D.
Pincini
,
Y.
Shi
,
Y.
Tsujimoto
,
K.
Yamaura
,
M. Moretti
Sala
,
J.
Van Den Brink
,
A. d.
Christianson
,
D. F.
Mcmorrow
Abstract: The temperature dependence of the excitation spectrum in NaOsO3 through its metal-to-insulator transition (MIT) at 410 K has been investigated using resonant inelastic x-ray scattering at the Os L3 edge. High-resolution (ΔE∼56 meV) measurements show that the well-defined, low-energy magnons in the insulating state weaken and dampen upon approaching the metallic state. Concomitantly, a broad continuum of excitations develops which is well described by the magnetic fluctuations of a nearly antiferromagnetic Fermi liquid. By revealing the continuous evolution of the magnetic quasiparticle spectrum as it changes its character from itinerant to localized, our results provide unprecedented insight into the nature of the MIT in NaOsO3.
|
May 2018
|
|
I16-Materials and Magnetism
|
Diamond Proposal Number(s):
[14646]
Abstract: We report the observation of parametrically down-converted x-ray signal photons at photon energies that
correspond to idler photons at optical wavelengths. The count-rate dependence on the angles of the input
beam and of the detector and on the slit sizes agrees with theory within the experimental uncertainties. The
nonlinear susceptibility, which we calculated from the measured efficiencies, is comparable to the nonlinear
susceptibility evaluated from the measurements of x-ray and optical wave mixing. The results of the present
Letter advance the development of a spectroscopy method for probing valence-electron charges and the
microscopic optical response of crystals with atomic-scale resolution.
|
Dec 2017
|
|
I11-High Resolution Powder Diffraction
|
Peter J. E. M.
Van Der Linden
,
Marco
Moretti Sala
,
Christian
Henriquet
,
Matteo
Rossi
,
Kenya
Ohgushi
,
François
Fauth
,
Laura
Simonelli
,
Carlo
Marini
,
Edmundo
Fraga
,
Claire
Murray
,
Jonathan
Potter
,
Michael
Krisch
Diamond Proposal Number(s):
[14463]
Abstract: We have developed a helium gas flow cryostat for use on synchrotron tender to hard X-ray beamlines. Very efficient sample cooling is achieved because the sample is placed directly in the cooling helium flow on a removable sample holder. The cryostat is compact and easy to operate; samples can be changed in less than 5 min at any temperature. The cryostat has a temperature range of 2.5–325 K with temperature stability better than 0.1 K. The very wide optical angle and the ability to operate in any orientation mean that the cryostat can easily be adapted for different X-ray techniques. It is already in use on different beamlines at the European Synchrotron Radiation Facility (ESRF), ALBA Synchrotron Light Facility (ALBA), and Diamond Light Source (DLS) for inelastic X-ray scattering, powder diffraction, and X-ray absorption spectroscopy. Results obtained at these beamlines are presented here.
|
Nov 2016
|
|
|
|
Abstract: Using resonant magnetic x-ray scattering we address the unresolved nature of the magnetic ground state and the low-energy effective Hamiltonian of Sm2Ir2O7, a prototypical pyrochlore iridate with a finite temperature metal-insulator transition. Through a combination of elastic and inelastic measurements, we show that the magnetic ground state is an all-in–all-out (AIAO) antiferromagnet. The magnon dispersion indicates significant electronic correlations and can be well described by a minimal Hamiltonian that includes Heisenberg exchange [J=27.3(6) meV ] and Dzyaloshinskii-Moriya interactions [D=4.9(3) meV ], which provides a consistent description of the magnetic order and excitations. In establishing that Sm2Ir2 O7 has the requisite inversion symmetry preserving AIAO magnetic ground state, our results support the notion that pyrochlore iridates may host correlated Weyl semimetals.
|
Jul 2016
|
|
