I21-Resonant Inelastic X-ray Scattering (RIXS)
|
Abstract: Spinel oxides are well-known functional materials but rarely show superconductivity. Recently, emergent superconductivity was discovered in
MgTi
2
O
4
, which is attributed to the increase of electron doping and the suppression of orbital order. Here, we utilized Ti
L
-edge resonant inelastic x-ray scattering to study the orbital excitations in superconducting (SC) and insulating
MgTi
2
O
4
films. We find that the spectral weight of orbital excitations is enhanced and the energy of
t
2
g
intraband excitation is softened in the SC film compared to the insulating one, suggesting higher electron doping and a suppressed orbital order gap in the SC sample. These observations were further supported by our multiplet calculations using the minimal two-site model. Our results provide spectroscopic evidence for the competition between orbital order and superconductivity in
MgTi
2
O
4
and shed light on searching for novel superconductors in spinel oxides.
|
Mar 2023
|
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I15-Extreme Conditions
I19-Small Molecule Single Crystal Diffraction
|
David M.
Jarvis
,
Matthew J.
Coak
,
Hayrullo
Hamidov
,
Charles R. S.
Haines
,
Giulio I.
Lampronti
,
Cheng
Liu
,
Shiyu
Deng
,
Dominik
Daisenberger
,
David R.
Allan
,
Mark R.
Warren
,
Andrew R.
Wildes
,
Siddharth S.
Saxena
Diamond Proposal Number(s):
[15949, 23524]
Abstract: FePS
3
is a layered magnetic van der Waals compound that undergoes a Mott insulator-metal transition under applied pressure. The transition has an associated change in the crystal symmetry and magnetic structure. Understanding the underlying physics of these transitions requires a detailed understanding of the crystal structure as a function of pressure. Two conflicting models have previously been proposed for the evolution of the structure with pressure. To settle the disagreement, we present a study of the pressure-dependent crystal structures using both single-crystal and powder x-ray diffraction measurements. We show unambiguously that the highest-pressure transition involves a collapse of the interplanar spacing, along with an increase in symmetry from a monoclinic to a trigonal space group, to the exclusion of other models. Our collected results are crucial for understanding high-pressure behavior in these materials and demonstrate a clear and complete methodology for exploring complex two-dimensional material structures under pressure.
|
Feb 2023
|
|
I15-1-X-ray Pair Distribution Function (XPDF)
I15-Extreme Conditions
|
Ge
Wang
,
Tengfei
Hu
,
Wenxuan
Zhu
,
Zhilun
Lu
,
Annette
Kleppe
,
Maria
Diaz Lopez
,
Antonio
Feteira
,
Derek C.
Sinclair
,
Zhengqian
Fu
,
Houbing
Huang
,
Dawei
Wang
,
Ian M.
Reaney
Diamond Proposal Number(s):
[21714, 27500]
Abstract: For the first time, the origin of large electrostrain in pseudocubic
BiFeO
3
-based ceramics is verified with direct structural evidence backed by appropriate simulations. We employ advanced structural and microstructural characterizations of
BiFeO
3
-based ceramics that exhibit large electrostrain (
>
0.4
%
) to reveal the existence of multiple, nanoscale local symmetries, dominantly tetragonal or orthorhombic, which have a common, averaged direction of polarization over larger, meso- or microscale regions. Phase-field simulations confirm the existence of local nanoscale symmetries, thereby providing a new vision for designing high-performance lead-free ceramics for high-strain actuators.
|
Feb 2023
|
|
I10-Beamline for Advanced Dichroism
|
Xiaodong
Xie
,
Kejing
Ran
,
Yizhou
Liu
,
Raymond
Fan
,
Wancong
Tan
,
Haonan
Jin
,
Manuel
Valvidares
,
Nicolas
Jaouen
,
Haifeng
Du
,
Gerrit
Van Der Laan
,
Thorsten
Hesjedal
,
Shilei
Zhang
Diamond Proposal Number(s):
[20437, 26148, 22629]
Abstract: We identify a three-dimensional skyrmion side-face state in chiral magnets that consists of a thin layer of modulated surface spirals and an array of phase-locked skyrmion screws. Such chiral spin structures lead to a characteristic X-shaped magnetic diffraction pattern in resonant elastic x-ray scattering, reminiscent of Photo 51 of the DNA double-helix diffraction. By measuring both thin plates and bulk
Cu
2
OSeO
3
crystals in the field-in-plane geometry, we unambiguously identify the modulated skyrmion strings by retrieving their chirality and helix angle. The breaking of the translational symmetry along the side faces suppresses the bulk-favored conical state, providing a stabilization mechanism for the skyrmion lattice phase that has been overlooked so far.
|
Feb 2023
|
|
I06-Nanoscience
|
Diamond Proposal Number(s):
[14135]
Abstract: The size of the orbital moment in
Fe
3
O
4
has been the subject of a long-standing and contentious debate. In this paper, we make use of ferromagnetic resonance (FMR) spectroscopy and x-ray magnetic circular dichroism (XMCD) to provide complementary determinations of the size of the orbital moment in “bulklike” epitaxial
Fe
3
O
4
films grown on yttria-stabilized zirconia (111) substrates. Annealing the 100 nm as-grown films to
1100
∘
C
in a reducing atmosphere improves the stoichiometry and microstructure of the films, allowing for bulklike properties to be recovered as evidenced by x-ray diffraction and vibrating sample magnetometry. In addition, in-plane angular FMR spectra exhibit a crossover from a fourfold symmetry to the expected sixfold symmetry of the (111) surface, together with an anomalous peak in the FMR linewidth at
∼
10
GHz; this is indicative of low Gilbert damping in combination with two-magnon scattering. For the bulklike annealed sample, a spectroscopic splitting factor
g
≈
2.18
is obtained using both FMR and XMCD techniques, providing evidence for the presence of a finite orbital moment in
Fe
3
O
4
.
|
Feb 2023
|
|
I05-ARPES
|
Edgar
Abarca Morales
,
Gesa-R.
Siemann
,
Andela
Zivanovic
,
Philip A. E.
Murgatroyd
,
Igor
Markovic
,
Brendan
Edwards
,
Chris A.
Hooley
,
Dmitry A.
Sokolov
,
Naoki
Kikugawa
,
Cephise
Cacho
,
Matthew D.
Watson
,
Timur K.
Kim
,
Clifford W.
Hicks
,
Andrew P.
Mackenzie
,
Phil D. C.
King
Diamond Proposal Number(s):
[27471, 28412]
Abstract: We report the evolution of the electronic structure at the surface of the layered perovskite
Sr
2
RuO
4
under large in-plane uniaxial compression, leading to anisotropic
B
1
g
strains of
ϵ
x
x
−
ϵ
y
y
=
−
0.9
±
0.1
%
. From angle-resolved photoemission, we show how this drives a sequence of Lifshitz transitions, reshaping the low-energy electronic structure and the rich spectrum of van Hove singularities that the surface layer of
Sr
2
RuO
4
hosts. From comparison to tight-binding modeling, we find that the strain is accommodated predominantly by bond-length changes rather than modifications of octahedral tilt and rotation angles. Our study sheds new light on the nature of structural distortions at oxide surfaces, and how targeted control of these can be used to tune density of state singularities to the Fermi level, in turn paving the way to the possible realization of rich collective states at the
Sr
2
RuO
4
surface.
|
Feb 2023
|
|
B23-Circular Dichroism
|
Abstract: High-resolution calorimetry has played a significant role in providing detailed information on phase transitions in liquid crystals. In particular, adiabatic scanning calorimetry (ASC), capable of providing simultaneous information on the temperature dependence of the specific enthalpy
h
(
T
)
and on the specific heat capacity
c
p
(
T
)
, has proven to be an important tool to determine the order of transitions and render high-resolution information on pretransitional thermal behavior. Here we report on ASC results on the compound 2,3′,4′,5′-tetrafluoro[1,1′-biphenyl]-4-yl 2,6-difluoro-4-(5-propyl-1,3-dioxan-2-yl) benzoate (DIO) and on mixtures with 4-[(4-nitrophenoxy)carbonyl]phenyl 2,4-dimethoxybenzoate (RM734). Both compounds exhibit a low-temperature ferroelectric nematic phase (
N
F
) and a high-temperature paraelectric nematic phase
(
N
)
. However, in DIO these two phases are separated by an intermediate phase (
N
x
). From the detailed data of
h
(
T
)
and
c
p
(
T
)
, we found that the intermediate phase was present in all the mixtures over the complete composition range, albeit with strongly decreasing temperature width for that phase with decreasing mole fraction of DIO (
x
DIO
). The
x
DIO
dependence on the transition temperatures for both transitions could be well described by a quadratic function. Both these transitions were weakly first order. The true latent heat of the
N
x
−
N
transition of DIO was as low as
L
=
0.0075
±
0.0005
J
/
g
and
L
=
0.23
±
0.03
J
/
g
for the
N
F
−
N
x
transition, which is about twice the previously reported value of 0.115 J/g for the
N
F
−
N
transition in RM734. In the mixtures both transition latent heats decrease gradually with decreasing
x
DIO
. At all the
N
x
−
N
transitions pretransition fluctuation effects are absent and these transitions are purely but very weakly first order. As in RM734 the transition from the
N
F
to the higher-temperature phase exhibits substantial pretransitional behavior, in particular, in the high-temperature phase. Power-law analysis of
c
p
(
T
)
resulted in an effective critical exponent
α
=
0.88
±
0.1
for DIO and this value decreased in the mixtures with decreasing
x
DIO
toward
α
=
0.50
±
0.05
reported for RM734. Ideal mixture analysis of the phase diagram was consistent with ideal mixture behavior provided the total transition enthalpy change was used in the analysis.
|
Jan 2023
|
|
I10-Beamline for Advanced Dichroism
|
Diamond Proposal Number(s):
[23784]
Open Access
Abstract: Magnetic skyrmions (skyrmions hereafter) are magnetization configurations, whose topological robustness and nanoscale size have led to speculation that they could find use as a next-generation information carrier. Skyrmions have been observed in magnetic multilayer materials that are thin compared to the radius of a skyrmion, and chiral cubic single crystals that can be far larger than any characteristic skyrmion scale. In these single crystals, one would expect that skyrmions could exhibit interesting three-dimensional (3D) characteristics. Here, the symmetry of the micromagnetic free energy is investigated. This symmetry permits a complex 3D modulation of a skyrmion string, which we show to be a requirement of a skyrmion coexisting with the conical state. We discuss the implications of this modulation with respect to Thiele's equation and interskyrmion interactions. Further to this internal modulation, we study theoretically and show experimentally that the strings themselves must contort towards the surfaces of their confining crystals.
|
Dec 2022
|
|
|
Abstract: The Bragg diffraction of neutrons and x rays are well suited to the task of determining the distribution of magnetization in crystals. Applications of the two techniques proceed by contrasting observed intensities with intensities calculated with a specific model, and changing the model as need be to achieve satisfactory agreement. An all-in–all-out (AIAO) magnetic configuration of magnetic dipoles on a cubic face-centered lattice with networks of corner-sharing tetrahedra is often mentioned in the context of pyrochlore oxides, for example, but the corresponding neutron and x-ray-diffraction patterns appear to not have been calculated. Our results for patterns of Bragg spots from an AIAO magnetic configuration defined by a magnetic space group are symmetry informed and yield exact reflection conditions. Specifically, a long-range order of magnetic dipoles is forbidden in our model. Bulk properties arise from higher-order multipoles that include quadrupoles and octupoles. Bragg spots that exclude all magnetic multipoles other than an octupole have been discovered, and they can be observed by both neutron diffraction and resonant x-ray diffraction. All magnetic multipoles allowed in diffraction by cerium ions
(
4
f
1
)
are presented in terms of coefficients in a well-documented and unusual magnetic ground state. Symmetry of the cerium site in the cubic structure constrains the coefficients. Our scattering amplitudes have an application in both neutron- and x-ray diffraction experiments on
Ce
2
Zr
2
O
7
, for example, and searches for the sought-after cerium octupole. Also presented for future use is a result for the total, energy-integrated magnetic neutron-scattering intensity by a powder sample.
|
Dec 2022
|
|
I10-Beamline for Advanced Dichroism
|
Margaret R.
Mccarter
,
Kook Tae
Kim
,
Vladimir A.
Stoica
,
Sujit
Das
,
Christoph
Klewe
,
Elizabeth P.
Donoway
,
David M.
Burn
,
Padraic
Shafer
,
Fanny
Rodolakis
,
Mauro A. p.
Gonçalves
,
Fernando
Gómez-Ortiz
,
Jorge
Íñiguez
,
Pablo
García-Fernández
,
Javier
Junquera
,
Stephen W.
Lovesey
,
Gerrit
Van Der Laan
,
Se Young
Park
,
John W.
Freeland
,
Lane W.
Martin
,
Dong Ryeol
Lee
,
Ramamoorthy
Ramesh
Diamond Proposal Number(s):
[24797]
Abstract: An escalating challenge in condensed-matter research is the characterization of emergent order-parameter nanostructures such as ferroelectric and ferromagnetic skyrmions. Their small length scales coupled with complex, three-dimensional polarization or spin structures makes them demanding to trace out fully. Resonant elastic x-ray scattering (REXS) has emerged as a technique to study chirality in spin textures such as skyrmions and domain walls. It has, however, been used to a considerably lesser extent to study analogous features in ferroelectrics. Here, we present a framework for modeling REXS from an arbitrary arrangement of charge quadrupole moments, which can be applied to nanostructures in materials such as ferroelectrics. With this, we demonstrate how extended reciprocal space scans using REXS with circularly polarized x rays can probe the three-dimensional structure and chirality of polar skyrmions. Measurements, bolstered by quantitative scattering calculations, show that polar skyrmions of mixed chirality coexist, and that REXS allows valuation of relative fractions of right- and left-handed skyrmions. Our quantitative analysis of the structure and chirality of polar skyrmions highlights the capability of REXS for establishing complex topological structures toward future application exploits.
|
Dec 2022
|
|