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.
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Feb 2023
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B23-Circular Dichroism
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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
|
|
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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.
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Dec 2022
|
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I10-Beamline for Advanced Dichroism
|
Diamond Proposal Number(s):
[10207]
Open Access
Abstract: X-ray magnetic circular dichroism (XMCD), which by virtue of the sum rules provides element-specific spin and orbital moments, is obtained from the difference between two polarized spectra by reversing the direction of either the light helicity or the applied magnetic field. Usually, it is tacitly assumed that these two spectra are obtained using the same absolute degree of light and magnetic polarization. This is, however, not always possible and depends on circumstances that can be beyond control. First, we recapitulate the conventional XMCD sum rule method to obtain the values of the moments and emphasize some of the complications in the case of the rare-earth
M
4
,
5
edges, such as the presence of strong core-hole
j
j
overlap, linear dichroism, and magnetic dipole term
⟨
T
z
⟩
. Instead, we propose an alternative method. Using the individual polarized x-ray absorption spectra obtained at the Ho and Dy
M
5
edges, where each of the
Δ
J
=
−
1
,
0
, and
+
1
transitions are separated by
∼
2
eV in photon energy, we are able to determine independently the degree of circular dichroism in a single spectrum. Since light is a transverse wave, we need to include, apart from the circular dichroism, also a linear dichroism contribution in order to fit the circularly polarized spectra. In the measurements on paramagnetic rare-earth dopants it was found that reversing the field produces the same degree of circular dichroism, while reversing the helicity yields a
∼
20% difference in the degree of circular dichroism.
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Dec 2022
|
|
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.
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Dec 2022
|
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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.
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Dec 2022
|
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I10-Beamline for Advanced Dichroism
|
N.-J.
Steinke
,
S. L.
Zhang
,
P. J.
Baker
,
L. B.
Duffy
,
F.
Kronast
,
J.
Krieger
,
Z.
Salman
,
T.
Prokscha
,
A.
Suter
,
S.
Langridge
,
Gerrit
Van Der Laan
,
T.
Hesjedal
Diamond Proposal Number(s):
[11503]
Abstract: Chromium-doped
Sb
2
Te
3
is a magnetic topological insulator (MTI), which belongs to the
(
Sb
,
Bi
)
2
(
Se
,
Te
)
3
family. When doped with the transition metals V, Cr, and Mn this family displays long-range ferromagnetic order above liquid nitrogen temperature and is currently intensely explored for quantum device applications. Despite the large magnetic ordering temperature, the experimental observation of dissipationless electrical transport channels, i.e., the quantum anomalous Hall effect, is limited in these materials to temperatures below
≈
2
K. Inhomogeneities in the MTI have been identified as a major concern, affecting the coupling between the Dirac states and the magnetic dopants. Nevertheless, details on the local magnetic order in these materials are not well understood. Here, we report the study of the magnetic correlations in thin films using a combination of muon spin relaxation
(
μ
SR
)
, and magnetic soft x-ray spectroscopy and imaging.
μ
SR
provides two key quantities for understanding the microscopic magnetic behavior: The magnetic volume fraction, i.e., the percentage of the material that is ferromagnetically ordered, and the relaxation rate, which is sensitive to the magnetic static
(
≈
μ
s
)
and dynamic disorder. By choosing different implantation depths for the muons, one can further discriminate between near-surface and bulk properties. No evidence for a surface enhancement of the magnetic ordering is observed, but, instead, we find evidence of small magnetically ordered clusters in a paramagnetic background, which are coupled. The significant magnetic field shift that is present in all samples indicates a percolation transition that proceeds through the formation and growth of magnetically ordered spin clusters. We further find that fluctuations are present even at low temperatures, and that there appears to be a transition between superparamagnetism and superferromagnetism.
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Dec 2022
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B16-Test Beamline
|
Diamond Proposal Number(s):
[21446]
Abstract: A new Fano profile of a flat line is achieved experimentally by manipulating the relative amplitude of the continuum path, when
q
takes the pure imaginary number of
−
i
in the x-ray regime. The underlying mechanism is that the interference term in the scattering will cancel the discrete term exactly. This new Fano profile renders only an observable continuum along with an invisible response to the discrete state of atomic resonance. The results suggest not only a different strategy to invisibility studies which provides a possible tool to identify weaker structures hidden by the strong white line, but also a new scenario to enrich the manipulations of two-path interference and nonlinear Fano resonance.
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Nov 2022
|
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I10-Beamline for Advanced Dichroism
|
Diamond Proposal Number(s):
[16043, 17612]
Open Access
Abstract: Magnetic diffraction in combination with x-ray detected ferromagnetic resonance (DFMR) is a powerful technique for performing time-resolved measurements on individual spin textures. Here, we study the ferromagnetic resonance (FMR) modes of both the conical and field-polarized phases in the chiral magnet
Cu
2
OSeO
3
. Following the identification of the FMR modes at different temperatures using broadband vector network analyzer FMR, we use DFMR on the crystalline (001) Bragg peak to reveal the time-dependent spin configurations of the selected FMR modes. By being able to measure both the amplitude and phase response of the spin system across the resonance, a continuous phase advance (of
180
∘
) in the conical mode and a phase lag (of
180
∘
) in the field-polarized mode is found. By performing dynamic measurements in the conical phase as a function of the linear polarization angle of the x rays, i.e., successively probing the dynamics of the moments, we find an inversion of the dynamics along the conical axis upon inverting the applied field direction. By allowing for time-resolved measurements of the phase and amplitude of individual magnetic phases, DFMR opens up new opportunities for obtaining a deeper understanding of the complex dynamics of chiral magnets.
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Nov 2022
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I09-Surface and Interface Structural Analysis
|
Diamond Proposal Number(s):
[24219, 31069]
Abstract: Ga
2
O
3
is emerging as a promising wide band-gap semiconductor for high-power electronics and deep ultraviolet optoelectronics. It is highly desirable to dope it with controllable carrier concentrations for different device applications. This work reports a combined photoemission spectroscopy and theoretical calculation study on the electronic structure of Si doped
Ga
2
O
3
films with carrier concentration varying from
4.6
×
10
18
c
m
−
3
to
2.6
×
10
20
c
m
−
3
. Hard x-ray photoelectron spectroscopy was used to directly measure the widening of the band gap as a result of occupation of conduction band and band-gap renormalization associated with many-body interactions. A large band-gap renormalization of 0.3 eV was directly observed in heavily doped
Ga
2
O
3
. Supplemented with hybrid density functional theory calculations, we demonstrated that the band-gap renormalization results from the decrease in energy of the conduction band edge driven by the mutual electrostatic interaction between added electrons. Moreover, our work reveals that Si is a superior dopant over Ge and Sn, because
Si
3
s
forms a resonant donor state above the conduction band minimum, leaving the host conduction band mostly unperturbed and a high mobility is maintained though the doping level is high. Insights of the present work have significant implications in doping optimization of
Ga
2
O
3
and realization of optoelectronic devices.
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Nov 2022
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