|
|
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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I08-Scanning X-ray Microscopy beamline (SXM)
|
Dawn M.
Buchanan
,
Laura
Newsome
,
Jonathan R.
Lloyd
,
Majid
Kazemian
,
Burkhard
Kaulich
,
Tohru
Araki
,
Heath
Bagshaw
,
John
Waters
,
Gerrit
Van Der Laan
,
Alpha
N’diaye
,
Victoria S.
Coker
Diamond Proposal Number(s):
[17626]
Open Access
Abstract: Cobalt is an essential element for life and plays a crucial role in supporting the drive to clean energy, due to its importance in rechargeable batteries. Co is often associated with Fe in the environment, but the fate of Co in Fe-rich biogeochemically-active environments is poorly understood. To address this, synchrotron-based scanning X-ray microscopy (SXM) was used investigate the behaviour of cobalt at the nanoscale in Co-Fe(III)-oxyhydroxides undergoing microbial reduction. SXM can assess spatial changes in metal speciation and organic compounds helping to elucidate the electron transfer processes occurring at the cell-mineral interface and inform on the fate of cobalt in redox horizons. G. sulfurreducens was used to reduce synthetic Co-ferrihydrite as an analogue of natural cobalt-iron-oxides. Magnetite [Fe(II)/Fe(III)3O4] production was confirmed by powder X-ray diffraction (XRD), SXM and X-ray magnetic circular dichroism (XMCD) data, where best fits of the latter suggested Co-bearing magnetite. Macro-scale XAS techniques suggested Co(III) reduction occurred and complementary SXM at the nanoscale, coupled with imaging, found localised biogenic Co(III) reduction at the cell-mineral interface via direct contact with outer membrane cytochromes. No discernible localised changes in Fe speciation were detected in the reordered cobalt-iron-oxides that were formed and at the end point of the experiment only 11% Co and 1.5% Fe had been solubilised. The solid phase retention, alongside the highly localised and preferential cobalt bioreduction observed at the nanoscale is consistent with retention of Co in redox zones. This work improves our fundamental molecular-scale understanding of the fate of Co in complex environmental systems and supports the development of biogenic Co-doped magnetite for industrial applications from drug delivery systems to magnetic recording media.
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May 2022
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I06-Nanoscience
|
G.
Awana
,
R.
Fujita
,
A.
Frisk
,
P.
Chen
,
Q.
Yao
,
A. J.
Caruana
,
C. J.
Kinane
,
N.-J.
Steinke
,
S.
Langridge
,
P.
Olalde-Velasco
,
S. S.
Dhesi
,
G.
Van Der Laan
,
X. F.
Kou
,
S. L.
Zhang
,
T.
Hesjedal
,
D.
Backes
Diamond Proposal Number(s):
[23748]
Open Access
Abstract: An elegant approach to overcome the intrinsic limitations of magnetically doped topological insulators is to bring a topological insulator in direct contact with a magnetic material. The aspiration is to realize the quantum anomalous Hall effect at high temperatures where the symmetry-breaking magnetic field is provided by a proximity-induced magnetization at the interface. Hence, a detailed understanding of the interfacial magnetism in such heterostructures is crucial, yet its distinction from structural and magnetic background effects is a rather nontrivial task. Here, we combine several magnetic characterization techniques to investigate the magnetic ordering in
MnTe
/
Bi
2
Te
3
heterostructures. A magnetization profile of the layer stack is obtained using depth-sensitive polarized neutron reflectometry. The magnetic constituents are characterized in more detail using element-sensitive magnetic x-ray spectroscopy. Magnetotransport measurements provide additional information about the magnetic transitions. We find that the supposedly antiferromagnetic MnTe layer does not exhibit an x-ray magnetic linear dichroic signal, raising doubt that it is in its antiferromagnetic state. Instead, Mn seems to penetrate into the surface region of the
Bi
2
Te
3
layer. Furthermore, the interface between MnTe and
Bi
2
Te
3
is not abrupt, but extending over
∼
2.2
nm. These conditions are the likely reason that we do not observe proximity-induced magnetization at the interface. Our findings illustrate the importance of not solely relying on one single technique as proof for proximity-induced magnetism at interfaces. We demonstrate that a holistic, multitechnique approach is essential to gain a more complete picture of the magnetic structure in which the interface is embedded.
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May 2022
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I10-Beamline for Advanced Dichroism
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Kook Tae
Kim
,
Margaret R.
Mccarter
,
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
,
Sandhya
Susarla
,
Stephen W.
Lovesey
,
Gerrit
Van Der Laan
,
Se Young
Park
,
Lane W.
Martin
,
John W.
Freeland
,
Ramamoorthy
Ramesh
,
Dong Ryeol
Lee
Diamond Proposal Number(s):
[24797]
Open Access
Abstract: Resonant elastic X-ray scattering (REXS) offers a unique tool to investigate solid-state systems providing spatial knowledge from diffraction combined with electronic information through the enhanced absorption process, allowing the probing of magnetic, charge, spin, and orbital degrees of spatial order together with electronic structure. A new promising application of REXS is to elucidate the chiral structure of electrical polarization emergent in a ferroelectric oxide superlattice in which the polarization vectors in the REXS amplitude are implicitly described through an anisotropic tensor corresponding to the quadrupole moment. Here, we present a detailed theoretical framework and analysis to quantitatively analyze the experimental results of Ti L-edge REXS of a polar vortex array formed in a PbTiO3/SrTiO3 superlattice. Based on this theoretical framework, REXS for polar chiral structures can become a useful tool similar to x-ray resonant magnetic scattering (XRMS), enabling a comprehensive study of both electric and magnetic REXS on the chiral structures.
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Apr 2022
|
|
I06-Nanoscience
|
X.
Gu
,
C.
Chen
,
W. S.
Wei
,
L. L.
Gao
,
J. Y.
Liu
,
X.
Du
,
D.
Pei
,
J. S.
Zhou
,
R. Z.
Xu
,
Z. X.
Yin
,
W. X.
Zhao
,
Y. D.
Li
,
C.
Jozwiak
,
A.
Bostwick
,
E.
Rotenberg
,
D.
Backes
,
L. S. I.
Veiga
,
S.
Dhesi
,
T.
Hesjedal
,
G.
Van Der Laan
,
H. F.
Du
,
W. J.
Jiang
,
Y. P.
Qi
,
G.
Li
,
W. J.
Shi
,
Z. K.
Liu
,
Y. L.
Chen
,
L. X.
Yang
Diamond Proposal Number(s):
[27482]
Abstract: Crystal geometry can greatly influence the emergent properties of quantum materials. As an example, the kagome lattice is an ideal platform to study the rich interplay between topology, magnetism, and electronic correlation. In this work, combining high-resolution angle-resolved photoemission spectroscopy and ab initio calculation, we systematically investigate the electronic structure of
X
Mn
6
Sn
6
(
X
=
Dy
,
Tb
,
Gd
,
Y
)
family compounds. We observe the Dirac fermion and the flat band arising from the magnetic kagome lattice of Mn atoms. Interestingly, the flat band locates in the same energy region in all compounds studied, regardless of their different magnetic ground states and
4
f
electronic configurations. These observations suggest a robust Mn magnetic kagome lattice across the
X
Mn
6
Sn
6
family, thus providing an ideal platform for the search for, and investigation of, new emergent phenomena in magnetic topological materials.
|
Apr 2022
|
|
I10-Beamline for Advanced Dichroism
|
Diamond Proposal Number(s):
[26148]
Open Access
Abstract: A major challenge in topological magnetism lies in the three-dimensional (3D) exploration of their magnetic textures. A recent focus has been the question of how 2D skyrmion sheets vertically stack to form distinct types of 3D topological strings. Being able to manipulate the vertical coupling should therefore provide a route to the engineering of topological states. Here, we present a new type of axially bound magnetic skyrmion string state in which the strings in two distinct materials are glued together across their interface. With quasi-tomographic resonant elastic X-ray scattering, the 3D skyrmion profiles before and after their binding across the interface were unambiguously determined and compared. Their attractive binding is accompanied by repulsive twisting; i.e., the coupled skyrmions mutually affect each other via a compensating twisting. This state exists in chiral magnet–magnetic thin film heterostructures, providing a new arena for the engineering of 3D topological phases.
|
Apr 2022
|
|
|
|
Cyril
Leveille
,
Erick
Burgos-Parra
,
Yanis
Sassi
,
Fernando
Ajejas
,
Valentin
Chardonnet
,
Emanuele
Pedersoli
,
Flavio
Capotondi
,
Giovanni
De Ninno
,
Francesco
Maccherozzi
,
Sarnjeet
Dhesi
,
David M.
Burn
,
Gerrit
Van Der Laan
,
Oliver S.
Latcham
,
Andrey V.
Shytov
,
Volodymyr V.
Kruglyak
,
Emmanuelle
Jal
,
Vincent
Cros
,
Jean-Yves
Chauleau
,
Nicolas
Reyren
,
Michel
Viret
,
Nicolas
Jaouen
Open Access
Abstract: Non-collinear spin textures in ferromagnetic ultrathin films are attracting a renewed interest fueled by possible fine engineering of several magnetic interactions, notably the interfacial Dzyaloshinskii-Moriya interaction. This allows for the stabilization of complex chiral spin textures such as chiral magnetic domain walls (DWs), spin spirals, and magnetic skyrmions among others. We report here on the behavior of chiral DWs at ultrashort timescale after optical pumping in perpendicularly magnetized asymmetric multilayers. The magnetization dynamics is probed using time-resolved circular dichroism in x-ray resonant magnetic scattering (CD-XRMS). We observe a picosecond transient reduction of the CD-XRMS, which is attributed to the spin current-induced coherent and incoherent torques within the continuously varying spin texture of the DWs. We argue that a specific demagnetization of the inner structure of the DW induces a flow of spins from the interior of the neighboring magnetic domains. We identify this time-varying change of the DW texture shortly after the laser pulse as a distortion of the homochiral Néel shape toward a transient mixed Bloch-Néel-Bloch texture along a direction transverse to the DW.
|
Mar 2022
|
|
|
|
Piush
Behera
,
Molly A.
May
,
Fernando
Gómez-Ortiz
,
Sandhya
Susarla
,
Sujit
Das
,
Christopher T.
Nelson
,
Lucas
Caretta
,
Shang-Lin
Hsu
,
Margaret R.
Mccarter
,
Benjamin H.
Savitzky
,
Edward S.
Barnard
,
Archana
Raja
,
Zijian
Hong
,
Pablo
García-Fernandez
,
Stephen W.
Lovesey
,
Gerrit
Van Der Laan
,
Peter
Ercius
,
Colin
Ophus
,
Lane W.
Martin
,
Javier
Junquera
,
Markus B.
Raschke
,
Ramamoorthy
Ramesh
Open Access
Abstract: Polar textures have attracted substantial attention in recent years as a promising analog to spin-based textures in ferromagnets. Here, using optical second-harmonic generation–based circular dichroism, we demonstrate deterministic and reversible control of chirality over mesoscale regions in ferroelectric vortices using an applied electric field. The microscopic origins of the chirality, the pathway during the switching, and the mechanism for electric field control are described theoretically via phase-field modeling and second-principles simulations, and experimentally by examination of the microscopic response of the vortices under an applied field. The emergence of chirality from the combination of nonchiral materials and subsequent control of the handedness with an electric field has far-reaching implications for new electronics based on chirality as a field-controllable order parameter.
|
Jan 2022
|
|
Theoretical Physics
|
Abstract: Rutile-type RuO2 likely supports a simple antiferromagnetic structure which can be verified by x-ray Bragg
diffraction. Three magnetic motifs that do not break translation symmetry are explored in calculations of amplitudes suitable for diffraction enhanced by tuning the primary x-ray energy to a ruthenium atomic resonance. Coupling to x-ray helicity through a charge-magnetic interference is common to all motifs, together with magnetic and charge intensities in quadrature in the rotated channel of polarization. Necessary conditions for these diffraction phenomena are a centrosymmetric crystal structure, null magnetic propagation vector, and absence of a linear magnetoelectric effect. Published x-ray diffraction data for RuO2 were analyzed by the authors against a
magnetic motif that does not satisfy the conditions. A polarized neutron study of antiferromagnetic domains can be achieved with a sample that meets the stated crystal and magnetic symmetries.
|
Jan 2022
|
|
I10-Beamline for Advanced Dichroism
|
Diamond Proposal Number(s):
[28727]
Open Access
Abstract: The low-temperature electronic structure of the van der Waals ferromagnet CrSiTe3 has been investigated. This ferromagnetic semiconductor has a magnetic bulk transition temperature of 33 K, which can reach up to 80 K in single- and few-layer flakes. X-ray absorption spectroscopy (XAS) and x-ray magnetic circular dichroism (XMCD) measurements, carried out at the Cr L2,3 and Te Mb edges on in vacuo cleaved single crystals, give strong evidence for hybridization-mediated super-exchange between the Cr atoms. The observed chemical shift in the XAS, as well as the comparison of the XMCD with the calculated Cr L2,3 multiplet spectra, confirm a strongly covalent bond between the Cr 3d(eg) and Te 5p states. Application of the XMCD sum rules gives a non-vanishing orbital moment, supporting a partial occupation of the eg states, apart from the t2g. Also, the presence of a non-zero XMCD signal at the Te Mb edge confirms a Te 5p spin polarization due to mixing with the Cr eg bonding states. The results strongly suggest that superexchange, instead of the previously suggested single ion anisotropy, is responsible for the low-temperature ferromagnetic ordering of 2D materials such as CrSiTe3 and CrGeTe3. This demonstrates the interplay between electron correlation and ferromagnetism in insulating two-dimensional materials.
|
Dec 2021
|
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