I16-Materials and Magnetism
|
Jian-Rui
Soh
,
Irián
Sánchez-Ramírez
,
Xupeng
Yang
,
Jinzhao
Sun
,
Ivica
Zivkovic
,
J. Alberto
Rodríguez-Velamazán
,
Oscar
Fabelo
,
Anne
Stunault
,
Alessandro
Bombardi
,
Christian
Balz
,
Manh Duc
Le
,
Helen C.
Walker
,
J. Hugo
Dil
,
Dharmalingam
Prabhakaran
,
Henrik M.
Ronnow
,
Fernando
De Juan
,
Maia G.
Vergniory
,
Andrew T.
Boothroyd
Diamond Proposal Number(s):
[20347]
Open Access
Abstract: In the rapidly expanding field of topological materials there is growing interest in systems whose topological electronic band features can be induced or controlled by magnetism. Magnetic Weyl semimetals, which contain linear band crossings near the Fermi level, are of particular interest owing to their exotic charge and spin transport properties. Up to now, the majority of magnetic Weyl semimetals have been realized in ferro- or ferrimagnetically ordered compounds, but a disadvantage of these materials for practical use is their stray magnetic field which limits the minimum size of devices. Here we show that Weyl nodes can be induced by a helical spin configuration, in which the magnetization is fully compensated. Using a combination of neutron diffraction and resonant elastic x-ray scattering, we find that below TN = 14.5 K the Eu spins in EuCuAs develop a planar helical structure which induces two quadratic Weyl nodes with Chern numbers C = ±2 at the A point in the Brillouin zone.
|
Jan 2024
|
|
I16-Materials and Magnetism
|
Diamond Proposal Number(s):
[27353]
Open Access
Abstract: Magnetic topological insulators and semimetals are a class of crystalline solids whose properties are strongly influenced by the coupling between non-trivial electronic topology and magnetic spin configurations. Such materials can host exotic electromagnetic responses. Among these are topological insulators with certain types of antiferromagnetic order which are predicted to realize axion electrodynamics. Here we investigate the highly unusual helimagnetic phases recently reported in EuIn2As2, which has been identified as a candidate for an axion insulator. Using resonant elastic x-ray scattering we show that the two types of magnetic order observed in EuIn2As2 are spatially uniform phases with commensurate chiral magnetic structures, ruling out a possible phase-separation scenario, and we propose that entropy associated with low energy spin fluctuations plays a significant role in driving the phase transition between them. Our results establish that the magnetic order in EuIn2As2 satisfies the symmetry requirements for an axion insulator.
|
Jun 2023
|
|
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
|
|
I05-ARPES
I11-High Resolution Powder Diffraction
|
J.-R.
Soh
,
F.
De Juan
,
M. G.
Vergniory
,
N. B. M.
Schröter
,
M. C.
Rahn
,
D. Y.
Yan
,
J.
Jiang
,
M.
Bristow
,
P. A.
Reiss
,
J. N.
Blandy
,
Y. F.
Guo
,
Y. G.
Shi
,
T. K.
Kim
,
A.
Mccollam
,
S. H.
Simon
,
Y.
Chen
,
A. I.
Coldea
,
A. T.
Boothroyd
Diamond Proposal Number(s):
[19234, 18786]
Abstract: We report theoretical and experimental evidence that
EuCd
2
As
2
in magnetic fields greater than 1.6 T applied along the
c
axis is a Weyl semimetal with a single pair of Weyl nodes. Ab initio electronic structure calculations, verified at zero field by angle-resolved photoemission spectra, predict Weyl nodes with wave vectors
k
=
(
0
,
0
,
±
0.03
)
×
2
π
/
c
at the Fermi level when the Eu spins are fully aligned along the
c
axis. Shubnikov–de Haas oscillations measured in fields parallel to
c
reveal a cyclotron effective mass of
m
∗
c
=
0.08
m
e
and a Fermi surface of extremal area
A
ext
=
0.24
nm
−
2
, corresponding to 0.1% of the area of the Brillouin zone. The small values of
m
∗
c
and
A
ext
are consistent with quasiparticles near a Weyl node. The identification of
EuCd
2
As
2
as a model Weyl semimetal opens the door to fundamental tests of Weyl physics.
|
Nov 2019
|
|
I16-Materials and Magnetism
|
Diamond Proposal Number(s):
[14024]
Open Access
Abstract: We study the magnetic structure of the “stuffed” (Tb-rich) pyrochlore iridate Tb2+xIr2−xO7−y, using resonant elastic x-ray scattering (REXS). In order to disentangle contributions from Tb and Ir magnetic sublattices, experiments were performed at the Ir L3 and Tb M5 edges, which provide selective sensitivity to Ir 5d and Tb 4f magnetic moments, respectively. At the Ir L3 edge, we found the onset of long-range k = 0 magnetic order below TIr N ∼71K, consistent with the expected signal of all-in all-out (AIAO) magnetic order. Using a single-ion model to calculate REXS crosssections, we estimate an ordered magnetic moment of µIr 5d ≈ 0.34(3)µB at 5K. At the Tb M5 edge,long-range k = 0 magnetic order appeared below ∼ 40K, also consistent with an AIAO magnetic structure on the Tb site. Additional insight into the magnetism of the Tb sublattice is gleaned from measurements at the M5 edge in applied magnetic fields up to 6T, which is found to completely suppress the Tb AIAO magnetic order. In zero applied field, the observed gradual onset of the Tb sublattice magnetisation with temperature suggests that it is induced by the magnetic order on the Ir site. The persistence of AIAO magnetic order, despite the greatly reduced ordering temperature and moment size compared to stoichiometric Tb2Ir2O7, for which TIr N = 130K and µIr 5d = 0.56µB, indicates that stuffing could be a viable means of tuning the strength of electronic correlations, thereby potentially offering a new strategy to achieve topologically non-trivial band crossings in pyrochlore iridates.
|
May 2019
|
|
B18-Core EXAFS
|
J.
Sannigrahi
,
D. T.
Adroja
,
C.
Ritter
,
W.
Kockelmann
,
A. D.
Hillier
,
K. S.
Knight
,
A. T.
Boothroyd
,
M.
Wakeshima
,
Y.
Hinatsu
,
J. F. W.
Mosselmans
,
S.
Ramos
Diamond Proposal Number(s):
[63810]
Abstract: Bulk studies have revealed a first-order valence phase transition in
Ba
2
PrRu
1
−
x
Ir
x
O
6
(
0.10
≤
x
≤
0.25
), which is absent in the parent compounds with
x
=
0
(
Pr
3
+
) and
x
=
1
(
Pr
4
+
), which exhibit antiferromagnetic order with transition temperatures
T
N
=
120
and 72 K, respectively. In the present study, we have used magnetization, heat capacity, neutron diffraction, inelastic neutron scattering, and x-ray absorption measurements to investigate the nature of the Pr ion in
x
=
0.1
. The magnetic susceptibility and heat capacity of
x
=
0.1
show a clear sign of the first-order valence phase transition below 175 K, where the Pr valence changes from 3+ to 4+. Neutron diffraction analysis reveals that
x
=
0.1
crystallizes in a monoclinic structure with space group
P
2
1
/
n
at 300 K, but below 175 K two phases coexist, the monoclinic having the Pr ion in a 3+ valence state and a cubic one (
F
m
¯
3
m
) having the Pr ion in a 4+ valence state. Clear evidence of an antiferromagnetic ordering of the Pr and Ru moments is found in the monoclinic phase of the
x
=
0.1
compound below 110 K in the neutron diffraction measurements. Meanwhile, the cubic phase remains paramagnetic down to 2 K, a temperature below which heat capacity and susceptibility measurements reveal a ferromagnetic ordering. High energy inelastic neutron scattering data reveal well-defined high-energy magnetic excitations near 264 meV at temperatures below the valence transition. Low energy INS data show a broad magnetic excitation centered at 50 meV above the valence transition, but four well-defined magnetic excitations at 7 K. The high energy excitations are assigned to the
Pr
4
+
ions in the cubic phase and the low energy excitations to the
Pr
3
+
ions in the monoclinic phase. Further direct evidence of the Pr valence transition has been obtained from the x-ray absorption spectroscopy. The results on the
x
=
0.1
compound are compared with those for
x
=
0
and 1.
|
May 2019
|
|
I10-Beamline for Advanced Dichroism - scattering
|
Abstract: The ground-state orbital occupancy of the Ru4+ ion in Ca2−xLaxRuO4[x=0, 0.05(1), 0.07(1), and 0.12(1)] was investigated by performing x-ray absorption spectroscopy (XAS) in the vicinity of the O K edge as a function of the angle between the incident beam and the surface of the single-crystal samples. A minimal model of the hybridization between the O 2p states probed at the K edge and the Ru 4d orbitals was used to analyze the XAS data, allowing the ratio of hole occupancies nxy/nyz,zx to be determined as a function of doping and temperature. For the samples displaying a low-temperature insulating ground state (x≤0.07), nxy/nyz,zx is found to increase significantly with increasing doping, with increasing temperature acting to further enhance nxy/nyz,zx. For the x=0.12 sample, which has a metallic ground state, the XAS spectra are found to be independent of temperature and not to be describable by the minimal hybridization model, while being qualitatively similar to the spectra displayed by the x≤0.07 samples above their insulating to metallic transitions. To understand the origin of the evolution of the electronic structure of Ca2−xLaxRuO4 across its phase diagram, we have performed theoretical calculations based on a model Hamiltonian, comprising electron-electron correlations, crystal field Δ, and spin-orbit coupling λ, of a Ru-O-Ru cluster, with realistic values used to parametrize the various interactions taken from the literature. Our calculations of the Ru hole occupancy as a function of Δ/λ provide an excellent description of the general trends displayed by the data. In particular they establish that the enhancement of nxy/nyz,zx is driven by significant modifications to the crystal field as the tetragonal distortion of the RuO6 octahedral changes from compressive to tensile with La doping. We have also used our model to show that the hole occupancy of the O 2p and Ru 4d orbitals displays the same general trend as a function of Δ/λ, thus validating the minimal hybridization model used to analyze the data. In essence, our results suggest that the predominant mechanism driving the emergence of the low-temperature metallic phase in La-doped Ca2RuO4 is the structurally induced redistribution of holes within the t2g orbitals, rather than the injection of free carriers.
|
Feb 2019
|
|
|
|
D. F.
Bowman
,
E.
Cemal
,
T.
Lehner
,
A. R.
Wildes
,
L.
Mangin-Thro
,
G. J.
Nilsen
,
M. J.
Gutmann
,
D. J.
Voneshen
,
D.
Prabhakaran
,
A. T.
Boothroyd
,
D. G.
Porter
,
C.
Castelnovo
,
K.
Refson
,
J. P.
Goff
Open Access
Abstract: Pyrochlore systems are ideally suited to the exploration of geometrical frustration in three dimensions, and their rich phenomenology encompasses topological order and fractional excitations. Classical spin ices provide the first context in which it is possible to control emergent magnetic monopoles, and anisotropic exchange leads to even richer behaviour associated with large quantum fluctuations. Whether the magnetic ground state of Yb2Ti2O7 is a quantum spin liquid or a ferromagnetic phase induced by a Higgs transition appears to be sample dependent. Here we have determined the role of structural defects on the magnetic ground state via the diffuse scattering of neutrons. We find that oxygen vacancies stabilise the spin liquid phase and the stuffing of Ti sites by Yb suppresses it. Samples in which the oxygen vacancies have been eliminated by annealing in oxygen exhibit a transition to a ferromagnetic phase, and this is the true magnetic ground state.
|
Feb 2019
|
|
I16-Materials and Magnetism
|
D.
Pincini
,
S.
Boseggia
,
R.
Perry
,
Ma. J.
Gutmann
,
S.
Ricco
,
L. S. I.
Veiga
,
C. D.
Dashwood
,
S. P.
Collins
,
G.
Nisbet
,
A.
Bombardi
,
D. G.
Porter
,
F.
Baumberger
,
A. T.
Boothroyd
,
D. F.
Mcmorrow
Diamond Proposal Number(s):
[15323, 15952, 15867, 18934]
Abstract: The chemical and magnetic structures of the series of compounds Ca2−xLaxRuO4 [x=0, 0.05(1), 0.07(1), 0.12(1)] have been investigated using neutron diffraction and resonant elastic x-ray scattering. Upon La doping, the low-temperature S-Pbca space group of the parent compound is retained in all insulating samples [x≤0.07(1)], but with significant changes to the atomic positions within the unit cell. These changes can be characterized in terms of the local
RuO6 octahedral coordination: with increasing doping, the structure, crudely speaking, evolves from an orthorhombic unit cell with compressed octahedra to a quasitetragonal unit cell with elongated ones. The magnetic structure on the other hand, is found to be robust, with the basic k=(0,0,0), b-axis antiferromagnetic order of the parent compound preserved below the critical La doping concentration of x≈0.11. The only effects of La doping on the magnetic structure are to suppress the A-centred mode, favoring the B mode instead, and to reduce the Néel temperature somewhat. Our results are discussed with reference to previous experimental reports on the effects of cation substitution on the d4 Mott insulator Ca2RuO4, as well as with regard to theoretical studies on the evolution of its electronic and magnetic structure. In particular, our results rule out the presence of a proposed ferromagnetic phase, and suggest that the structural effects associated with La substitution play an important role in the physics of the system.
|
Jul 2018
|
|
I11-High Resolution Powder Diffraction
|
Diamond Proposal Number(s):
[13284]
Abstract: We have performed inelastic neutron-scattering measurements on a powder sample of the superconductor lithium iron selenide hydroxide Li 1−x Fe x ODFe 1−y Se(x≃0.16,y≃0.02,T c =41K) . The spectrum shows an enhanced intensity below T c over an energy range of 0.64×2Δ
|
Oct 2016
|
|
