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Open Access
Abstract: The study of magnetic order in few- and monolayer van der Waals materials poses a challenge to the most commonly employed magnetic characterization techniques as they normally lack magnetic sensitivity and/or lateral resolution enabling their thickness-dependent probing. Here we demonstrate the usefulness of X-ray absorption spectroscopy (XAS) and X-ray magnetic circular dichroism (XMCD) measurements, carried out at the Cr L2,3 and Te M5 edges, for the study of the ferromagnetic semiconductor CrSiTe3 (CST) in the form of single- and few-layer flakes. By scanning the sample under the incident X-ray beam, a map of the exfoliated system was obtained, which reproduced the optical micrographs showing the detailed distribution and thicknesses of the flakes. In this way, XAS/XMCD was performed at selected sample areas, revealing the thickness-resolved spectroscopic and magnetic properties of the flakes, such as the spin and orbital magnetic moments. The spin moment, in line with the saturation field, is decreasing with film thickness, revealing a single-domain and out-of-plane magnetization for the thinnest films. For CST, the electronic properties are governed by the strong covalent bond between the Cr 3d(eg) and Te 5p states, giving rise to a superexchange scenario. We observed a gradually increasing ratio of orbital to spin moment for thinner flakes, which could be due to a further increase of the covalent mixing. Hysteresis loops were recorded at the Cr L3 edge, showing an open loop for 10 down to ∼3 layers, while the bulk shows a wasp-waist shaped loop. With the transition temperature from the soft to the hard ferromagnetic state decreasing with thickness, the monolayer shows a narrowed, closed loop at 10 K, suggesting its transition temperature >10 K. Our study demonstrates the unique capabilities of XAS/XMCD for the study of few-layer van der Waals magnets, correlation and ferromagnetism in CST.
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Jun 2022
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I10-Beamline for Advanced Dichroism
|
Diamond Proposal Number(s):
[19996]
Abstract: We report a comprehensive study on the magnetic ground state of
La
1.5
Ca
0.5
Co
O
4
combining single crystal neutron diffraction and resonant magnetic x-ray scattering at the
Co
L
2
,
3
edges. Three single-crystal samples obtained from the same boule were investigated exhibiting magnetic phase transitions from a high-temperature paramagnetic phase to an antiferromagnetic phase at
T
N
≈
52
K
. Single crystal neutron diffraction reveals that the crystal structure at room temperature shows an orthorhombic
A
-centered lattice but with
a
and
b
axes almost equal in length. The structural phase transition (charge-ordering-like) from the parent tetragonal cell takes place above 523 K into the space group
A
2
m
m
where two nonequivalent compressed and expanded
Co
O
6
octahedra are ordered showing a checkerboard pattern in the
a
b
plane. The charge segregation between the nonequivalent Co sites is about 0.4(1) electrons. Resonant magnetic x-ray reflections indexed as
(
1
/
4
,
1
/
4
,
0
)
t
,
(
1
/
4
,
1
/
4
,
1
)
t
, and
(
1
/
4
,
1
/
4
,
1
/
2
)
t
in the parent tetragonal cell were observed at low temperature at the
Co
L
2
,
3
-edge energy range. The resonant spectral shape, with a noticeable absence of any resonant enhancement at the
Co
L
2
edge, indicates that only
Co
2
+
-like ions participate in the magnetic ordering. The polarization analysis discloses that the orientation of Co magnetic moments is the same for the three magnetic orders and they are long-range ordered along the diagonal in the
a
b
plane of the parent tetragonal cell with a slight tilt in the
c
axis. Despite the onset temperatures for the three resonant magnetic reflections being the same,
≈
55
K
, different thermal behavior is observed between
(
1
/
4
,
1
/
4
,
1
/
2
)
t
and
(
1
/
4
,
1
/
4
,
L
)
t
(
L
=
integer
) reflections whose intensities maximize at different temperatures, suggesting the coexistence of two magnetic arrangements. Moreover, the intensity of the
(
1
/
4
,
1
/
4
,
1
/
2
)
t
magnetic reflection is at least ten times larger than that of the
(
1
/
4
,
1
/
4
,
L
)
t
(
L
=
integer
)
ones. On the other hand\, neutron diffraction measurements only detect a single type of antiferromagnetic ordering following the propagation vector
k
=
(
1
/
4
,
1
/
4
,
1
/
2
)
t
that involves half of the Co atoms in the unit cell. We conclude that the bulk magnetic order in
La
1.5
Ca
0.5
Co
O
4
corresponds then to this propagation vector
k
=
(
1
/
4
,
1
/
4
,
1
/
2
)
t
while
(
1
/
4
,
1
/
4
,
0
)
t
and
(
1
/
4
,
1
/
4
,
1
)
t
magnetic reflections correspond to a minority magnetic phase that must be due to changes in the oxygen stoichiometry near the surface.
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May 2021
|
|
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Moein
Adnani
,
Melissa
Gooch
,
Liangzi
Deng
,
Stefano
Agrestini
,
Javier
Herrero-Martin
,
Hung-Cheng
Wu
,
Chung-Kai
Chang
,
Taha
Salavati-Fard
,
Narayan
Poudel
,
Jose Luis
Garcia-Munoz
,
Samira
Daneshmandi
,
Zheng
Wu
,
Lars C.
Grabow
,
Yen-Chung
Lai
,
Hung-Duen
Yang
,
Eric
Pellegrin
,
Ching-Wu
Chu
Abstract: We have investigated the multiferroicity and magnetoelectric (ME) coupling in
Ho
Fe
W
O
6
. With a noncentrosymmetric polar structure (space group Pna
2
1
) at room temperature, this compound shows an onset of electric polarization with an antiferromagnetic ordering at the Néel temperature (
T
N
) of 17.8 K. The magnetic properties of the polycrystalline samples were studied by DC and AC magnetization and heat capacity measurements. The metamagnetic behavior at low temperatures was found to be directly related to the dielectric properties of the compound. In particular, field-dependent measurements of capacitance show a magnetocapacitance (MC) effect with double-hysteresis loop behavior in direct correspondence with the magnetization. Our x-ray diffraction results show the Pna
2
1
structure down to 8 K and suggest the absence of a structural phase transition across
T
N
. Soft x-ray absorption spectroscopy and soft x-ray magnetic circular dichroism (XMCD) measurements at the Fe
L
2
,
3
and Ho
M
4
,
5
edges revealed the oxidation state of Fe and Ho cations to be
3
+
. Fe
L
2
,
3
XMCD further shows that
Fe
3
+
cations are antiferromagnetically ordered in a noncollinear fashion with spins arranged
90
∘
with respect to each other. Our findings show that
Ho
Fe
W
O
6
is a type-II multiferroic exhibiting a MC effect. The observed MC effect and the change in polarization by the magnetic field, as well as their direct correspondence with magnetization, further support the strong ME coupling in this compound.
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Mar 2021
|
|
|
Yangkun
He
,
Gerhard H.
Fecher
,
Chenguang
Fu
,
Yu
Pan
,
Kaustuv
Manna
,
Johannes
Kroder
,
Ajay
Jha
,
Xiao
Wang
,
Zhiwei
Hu
,
Stefano
Agrestini
,
Javier
Herrero-Martin
,
Manuel
Valvidares
,
Yurii
Skourski
,
Walter
Schnelle
,
Plamen
Stamenov
,
Horst
Borrmann
,
Liu Hao
Tjeng
,
Rudolf
Schaefer
,
Stuart S. P.
Parkin
,
John Michael D.
Coey
,
Claudia
Felser
Open Access
Abstract: The development of high‐density magnetic recording media is limited by superparamagnetism in very small ferromagnetic crystals. Hard magnetic materials with strong perpendicular anisotropy offer stability and high recording density. To overcome the difficulty of writing media with a large coercivity, heat‐assisted magnetic recording was developed, rapidly heating the media to the Curie temperature Tc before writing, followed by rapid cooling. Requirements are a suitable Tc, coupled with anisotropic thermal conductivity and hard magnetic properties. Here, Rh2CoSb is introduced as a new hard magnet with potential for thin‐film magnetic recording. A magnetocrystalline anisotropy of 3.6 MJ m−3 is combined with a saturation magnetization of μ0Ms = 0.52 T at 2 K (2.2 MJ m−3 and 0.44 T at room temperature). The magnetic hardness parameter of 3.7 at room temperature is the highest observed for any rare‐earth‐free hard magnet. The anisotropy is related to an unquenched orbital moment of 0.42 μB on Co, which is hybridized with neighboring Rh atoms with a large spin–orbit interaction. Moreover, the pronounced temperature dependence of the anisotropy that follows from its Tc of 450 K, together with a thermal conductivity of 20 W m−1 K−1, make Rh2CoSb a candidate for the development of heat‐assisted writing with a recording density in excess of 10 Tb in.−2.
|
Oct 2020
|
|
|
D.-S.
Park
,
A. D.
Rata
,
I. V.
Maznichenko
,
S.
Ostanin
,
Y. L.
Gan
,
S.
Agrestini
,
G. J.
Rees
,
M.
Walker
,
J.
Li
,
J.
Herrero-Martin
,
G.
Singh
,
Z.
Luo
,
A.
Bhatnagar
,
Y. Z.
Chen
,
V.
Tileli
,
P.
Muralt
,
A.
Kalaboukhov
,
I.
Mertig
,
K.
Dörr
,
A.
Ernst
,
N.
Pryds
Open Access
Abstract: Complex oxides show extreme sensitivity to structural distortions and defects, and the intricate balance of competing interactions which emerge at atomically defined interfaces may give rise to unexpected physics. In the interfaces of non-magnetic complex oxides, one of the most intriguing properties is the emergence of magnetism which is sensitive to chemical defects. Particularly, it is unclear which defects are responsible for the emergent magnetic interfaces. Here, we show direct and clear experimental evidence, supported by theoretical explanation, that the B-site cation stoichiometry is crucial for the creation and control of magnetism at the interface between non-magnetic ABO3-perovskite oxides, LaAlO3 and SrTiO3. We find that consecutive defect formation, driven by atomic charge compensation, establishes the formation of robust perpendicular magnetic moments at the interface. Our observations propose a route to tune these emerging magnetoelectric structures, which are strongly coupled at the polar-nonpolar complex oxide interfaces.
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Jul 2020
|
|
|
Open Access
Abstract: Chromium telluride compounds are promising ferromagnets for proximity coupling to magnetic
topological insulators (MTIs) of the Cr-doped (Bi,Sb)2(Se,Te)3 class of materials as they share the same elements, thus simplifying thin film growth, as well as due to their compatible crystal structure.
Recently, it has been demonstrated that high quality (001)-oriented Cr2Te3 thin films with perpendicular
magnetic anisotropy can be grown on c-plane sapphire substrate. Here, we present a magnetic and
soft x-ray absorption spectroscopy study of the chemical and magnetic properties of Cr2Te3 thin films.
X-ray magnetic circular dichroism (XMCD) measured at the Cr L2,3 edges gives information about the
local electronic and magnetic structure of the Cr ions. We further demonstrate the overgrowth of Cr2Te3 (001) thin films by high-quality Cr-doped Sb2Te3 films. The magnetic properties of the layers have been characterized and our results provide a starting point for refining the physical models of the complex magnetic ordering in Cr2Te3 thin films, and their integration into advanced MTI heterostructures for quantum device applications.
|
Jul 2019
|
|
I10-Beamline for Advanced Dichroism
|
Diamond Proposal Number(s):
[17480]
Abstract: The combination of topological properties and magnetic order can lead to new quantum states and exotic physical phenomena, such as the quantum anomalous Hall (QAH) effect. The size of the magnetic gap in the topological surface states, key for the robust observation of the QAH state, scales with the magnetic moment of the doped three-dimensional topological insulator (TI). The pioneering transition-metal doped (Sb,Bi)2(Se,Te)3 thin films only allow for the observation of the QAH effect up to some 100 mK, despite the much higher magnetic ordering temperatures. On the other hand, high magnetic moment materials, such as rare-earth-doped (Sb,Bi)2(Se,Te)3 thin films, show large moments but no long-range magnetic order. Proximity coupling and interfacial effects, multiplied in artificial heterostructures, allowfor the engineering of the electronic and magnetic properties. Here, we show the successful growth of high-quality Dy:Bi2Te3/Cr:Sb2Te3 thin film heterostructures. Using x-ray magnetic spectroscopy we demonstrate that high transition temperature Cr:Sb2Te3 can introduce long-range magnetic order in high-moment Dy:Bi2Te3—upto a temperature of 17 K—in excellent agreement with first-principles calculations,which reveal the origin of the long-range magnetic order in a strong antiferromagnetic coupling between Dy and Cr magnetic moments at the interface extending over several layers. Engineered magnetic TI heterostructures may be an ideal materials platform for observing the QAH effect at liquid He temperatures and above.
|
May 2018
|
|
I10-Beamline for Advanced Dichroism
|
Abstract: Doping Mn1−xCoxWO4 with Co produces a rich magnetic phase diagram with a large number of ferroelectric phases. We present resonant x-ray magnetic scattering experiments in the known collinear AF4 phase of multiferroic Mn0.85Co0.15WO4 showing that Mn and Co spins point to different directions despite they randomly occupy the same crystallographic site. The resultant noncollinear exotic spin configuration is determined by a competition of Mn2+ and Co2+ magnetic anisotropies and demands a reexamination of the ferroelectric phase diagram of this model family beyond the previous average description of its magnetic orders.
|
Jun 2015
|
|
|
T. A. W.
Beale
,
G.
Beutier
,
S. R.
Bland
,
A.
Bombardi
,
L.
Bouchenoire
,
O.
Bunau
,
S.
Di Matteo
,
J.
Fernandez-Rodriguez
,
J. E.
Hamann-Borrero
,
J.
Herrero-Martin
,
V. L. R.
Jacques
,
R. D.
Johnson
,
A.
Juhin
,
T.
Matsumura
,
C.
Mazzoli
,
A. M.
Mulders
,
H.
Nakao
,
J.
Okamoto
,
S.
Partzsch
,
A. J.
Princep
,
V.
Scagnoli
,
J.
Strempfer
,
C.
Vecchini
,
Y.
Wakabayashi
,
H. C.
Walker
,
D.
Wermeille
,
Y.
Yamasaki
Open Access
Abstract: Resonant Elastic X-Ray Scattering (REXS) has played a fundamental role in understanding electronic properties and in revealing hidden order, local symmetries and exotic states realized in correlated solids. This article reports on some of the relevant scientific contributions and technical advances over the last 20 years, by providing a list of related publications produced by various groups all around the world. The given perspective is that of a group of young scientists involved at various times in the investigation of the beauty of electronic ordering by the REXS technique.
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Jun 2012
|
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