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Abstract: van der Waals materials provide a versatile toolbox for the emergence of new quantum phenomena and fabrication of functional heterostructures. Among them, the trihalide VI3 stands out for its unique magnetic and structural landscape. Here we investigate the spin and orbital magnetic degrees of freedom in the layered ferromagnet VI3 by means of temperature-dependent X-ray absorption spectroscopy and X-ray magnetic circular and linear dichroism. We detect localized electronic states and reduced magnetic dimensionality, due to electronic correlations. We furthermore provide experimental evidence of (a) an unquenched orbital magnetic moment (up to 0.66(7) μB/V atom) in the ferromagnetic state and (b) an instability of the orbital moment in the proximity of the spin reorientation transition. Our results support a coherent picture where electronic correlations give rise to a strong magnetic anisotropy and a large orbital moment and establish VI3 as a prime candidate for the study of orbital quantum effects.
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Jan 2024
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I05-ARPES
|
Federico
Mazzola
,
Stefan
Enzner
,
Philipp
Eck
,
Chiara
Bigi
,
Matteo
Jugovac
,
Iulia
Cojocariu
,
Vitaliy
Feyer
,
Zhixue
Shu
,
Gian Marco
Pierantozzi
,
Alessandro
De Vita
,
Pietro
Carrara
,
Jun
Fujii
,
Phil D. C.
King
,
Giovanni
Vinai
,
Pasquale
Orgiani
,
Cephise
Cacho
,
Matthew D.
Watson
,
Giorgio
Rossi
,
Ivana
Vobornik
,
Tai
Kong
,
Domenico
Di Sante
,
Giorgio
Sangiovanni
,
Giancarlo
Panaccione
Diamond Proposal Number(s):
[30171]
Open Access
Abstract: Engineering surfaces and interfaces of materials promises great potential in the field of heterostructures and quantum matter designers, with the opportunity to drive new many-body phases that are absent in the bulk compounds. Here, we focus on the magnetic Weyl kagome system Co3Sn2S2 and show how for the terminations of different samples the Weyl points connect differently, still preserving the bulk-boundary correspondence. Scanning tunneling microscopy has suggested such a scenario indirectly, and here, we probe the Fermiology of Co3Sn2S2 directly, by linking it to its real space surface distribution. By combining micro-ARPES and first-principles calculations, we measure the energy-momentum spectra and the Fermi surfaces of Co3Sn2S2 for different surface terminations and show the existence of topological features depending on the top-layer electronic environment. Our work helps to define a route for controlling bulk-derived topological properties by means of surface electrostatic potentials, offering a methodology for using Weyl kagome metals in responsive magnetic spintronics.
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Aug 2023
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|
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Open Access
Abstract: Polarization dependent x-ray absorption spectroscopy was used to study the magnetic ground state and the orbital occupation in bulk-phase VI3 van der Waals crystals below and above the ferromagnetic and structural transitions. X-ray natural linear dichroism and X-ray magnetic circular dichroism spectra acquired at the V L2,3 edges are compared against multiplet cluster calculations within the frame of the ligand field theory to quantify the intra-atomic electronic interactions at play and evaluate the effects of symmetry reduction occurring in a trigonally distorted VI6 unit. We observed a non zero linear dichroism proving the presence of an anisotropic charge density distribution around the V3+ ion due to the unbalanced hybridization between the Vanadium and the ligand states. Such hybridization acts as an effective trigonal crystal field, slightly lifting the degeneracy of the t22g ground state. However, the energy splitting associated to the distortion underestimates the experimental band gap, suggesting that the insulating ground state is stabilized by Mott correlation effects rather than via a Jahn-Teller mechanism. Our results clarify the role of the distortion in VI3 and establish a benchmark for the study of the spectroscopic properties of other van der Waals halides, including emerging 2D materials with mono and few-layers thickness, whose fundamental properties might be altered by reduced dimensions and interface proximity.
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Jun 2023
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I09-Surface and Interface Structural Analysis
|
Gian Marco
Pierantozzi
,
Alessandro
De Vita
,
Chiara
Bigi
,
Xin
Gui
,
Hung-Ju
Tien
,
Debashis
Mondal
,
Federico
Mazzola
,
Jun
Fujii
,
Ivana
Vobornik
,
Giovanni
Vinai
,
Alessandro
Sala
,
Cristina
Africh
,
Tien-Lin
Lee
,
Giorgio
Rossi
,
Tay-Rong
Chang
,
Weiwei
Xie
,
Robert J.
Cava
,
Giancarlo
Panaccione
Diamond Proposal Number(s):
[24968]
Open Access
Abstract: We unravel the interplay of topological properties and the layered (anti)ferromagnetic ordering in EuSn2P2, using spin and chemical selective electron and X-ray spectroscopies supported by first-principle calculations. We reveal the presence of in-plane long-range ferromagnetic order triggering topological invariants and resulting in the multiple protection of topological Dirac states. We provide clear evidence that layer-dependent spin-momentum locking coexists with ferromagnetism in this material, a cohabitation that promotes EuSn2P2 as a prime candidate axion insulator for topological antiferromagnetic spintronics applications.
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Jan 2022
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I09-Surface and Interface Structural Analysis
|
F.
Offi
,
K.
Yamauchi
,
S.
Picozzi
,
V.
Lollobrigida
,
A.
Verna
,
C.
Schlueter
,
T.-L.
Lee
,
A.
Regoutz
,
D. J.
Payne
,
A.
Petrov
,
G.
Vinai
,
G. M.
Pierantozzi
,
T.
Pincelli
,
G.
Panaccione
,
F.
Borgatti
Diamond Proposal Number(s):
[11322]
Abstract: Hybridization of electronic states and orbital symmetry in transition metal oxides are generally considered key ingredients in the description of both their electronic and magnetic properties. In the prototypical case of
La
0.65
Sr
0.35
MnO
3
(LSMO), a landmark system for spintronics applications, a description based solely on Mn
3
d
and O
2
p
electronic states is reductive. We thus analyzed elemental and orbital distributions in the LSMO valence band through a comparison between density functional theory calculations and experimental photoelectron spectra in a photon energy range from soft to hard x rays. We reveal a number of hidden contributions, arising specifically from La
5
p
, Mn
4
s
, and O
2
s
orbitals, considered negligible in previous analyses; our results demonstrate that all these contributions are significant for a correct description of the valence band of LSMO and of transition metal oxides in general.
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Oct 2021
|
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I06-Nanoscience (XPEEM)
|
Federico
Motti
,
G.
Vinai
,
Valentina
Bonanni
,
Vincent
Polewczyk
,
Paola
Mantegazza
,
Thomas
Forrest
,
Francesco
Maccherozzi
,
Stefania
Benedetti
,
Christian
Rinaldi
,
Matteo
Cantoni
,
Damiano
Cassese
,
Stefano
Prato
,
Sarnjeet S.
Dhesi
,
Giorgio
Rossi
,
Giancarlo
Panaccione
,
Piero
Torelli
Diamond Proposal Number(s):
[18810]
Abstract: A ferromagnetic (FM) thin film deposited on a substrate of
Pb
(
Mg
1
/
3
Nb
2
/
3
)
O
3
−
PbTiO
3
(PMN-PT) is an appealing heterostructure for the electrical control of magnetism, which would enable nonvolatile memories with ultralow-power consumption. Reversible and electrically controlled morphological changes at the surface of PMN-PT suggest that the magnetoelectric effects are more complex than the commonly used “strain-mediated” description. Here we show that changes in substrate morphology intervene in magnetoelectric coupling as a key parameter interplaying with strain. Magnetic-sensitive microscopy techniques are used to study magnetoelectric coupling in Fe/PMN-PT at different length scales, and compare different substrate cuts. The observed rotation of the magnetic anisotropy is connected to the changes in morphology, and mapped in the crack pattern at the mesoscopic scale. Ferroelectric polarization switching induces a magnetic field-free rotation of the magnetic domains at micrometer scale, with a wide distribution of rotation angles. Our results show that the relationship between the rotation of the magnetic easy axis and the rotation of the in-plane component of the electric polarization is not straightforward, as well as the relationship between ferroelectric domains and crack pattern. The understanding and control of this phenomenon is crucial to develop functional devices based on FM/PMN-PT heterostructures.
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Nov 2020
|
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I09-Surface and Interface Structural Analysis
|
G.
Vinai
,
C.
Bigi
,
A.
Rajan
,
M. D.
Watson
,
T.-L.
Lee
,
F.
Mazzola
,
S.
Modesti
,
S.
Barua
,
M.
Ciomaga Hatnean
,
G.
Balakrishnan
,
P. D. C.
King
,
P.
Torelli
,
G.
Rossi
,
G.
Panaccione
Diamond Proposal Number(s):
[21429]
Abstract: Among transition-metal dichalcogenides, mono and few-layers thick
VSe
2
has gained much recent attention following claims of intrinsic room-temperature ferromagnetism in this system, which have nonetheless proved controversial. Here, we address the magnetic and chemical properties of
Fe
/
VSe
2
heterostructure by combining element sensitive x-ray absorption spectroscopy and photoemission spectroscopy. Our x-ray magnetic circular dichroism results confirm recent findings that both native mono/few-layer and bulk
VSe
2
do not show intrinsic ferromagnetic ordering. Nonetheless, we find that ferromagnetism can be induced, even at room temperature, after coupling with a Fe thin film layer, with antiparallel alignment of the moment on the V with respect to Fe. We further consider the chemical reactivity at the
Fe
/
VSe
2
interface and its relation with interfacial magnetic coupling.
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Jan 2020
|
|
|
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Abstract: Magnetism in monolayer (ML) VSe2 has attracted broad interest in spintronics, while existing reports have not reached consensus. Using element-specific X-ray magnetic circular dichroism, a magnetic transition in ML VSe2 has been demonstrated at the contamination-free interface between Co and VSe2. Through interfacial hybridization with a Co atomic overlayer, a magnetic moment of about 0.4 μB per V atom in ML VSe2 is revealed, approaching values predicted by previous theoretical calculations. Promotion of the ferromagnetism in ML VSe2 is accompanied by its antiferromagnetic coupling to Co and a reduction in the spin moment of Co. In comparison to the absence of this interface-induced ferromagnetism at the Fe/ML MoSe2 interface, these findings at the Co/ML VSe2 interface provide clear proof that the ML VSe2, initially with magnetic disorder, is on the verge of magnetic transition.
|
Jul 2019
|
|
I09-Surface and Interface Structural Analysis
|
Anna
Regoutz
,
Alex M.
Ganose
,
Lars
Blumenthal
,
Christoph
Schlueter
,
Tien-Lin
Lee
,
Gregor
Kieslich
,
Anthony K.
Cheetham
,
Gwilherm
Kerherve
,
Ying-Sheng
Huang
,
Ruei-San
Chen
,
Giovanni
Vinai
,
Tommaso
Pincelli
,
Giancarlo
Panaccione
,
Kelvin H. L.
Zhang
,
Russell G.
Egdell
,
Johannes
Lischner
,
David O.
Scanlon
,
David J.
Payne
Diamond Proposal Number(s):
[12673]
Abstract: Theory and experiment are combined to gain an understanding of the electronic properties of OsO2, a poorly studied metallic oxide that crystallizes in the rutile structure. Hard and soft valence-band x-ray photoemission spectra of OsO2 single crystals are in broad agreement with the results of density-functional-theory calculations, aside from a feature shifted to high binding energy of the conduction band. The energy shift corresponds to the conduction electron plasmon energy measured by reflection electron energy loss spectroscopy. The plasmon satellite is reproduced by many-body perturbation theory.
|
Feb 2019
|
|
I09-Surface and Interface Structural Analysis
|
T.
Pincelli
,
V.
Lollobrigida
,
F.
Borgatti
,
A.
Regoutz
,
B.
Gobaut
,
C.
Schlueter
,
T.-L.
Lee
,
D. J.
Payne
,
M.
Oura
,
K.
Tamasaku
,
A. Y.
Petrov
,
P.
Graziosi
,
F. Miletto
Granozio
,
M.
Cavallini
,
G.
Vinai
,
R.
Ciprian
,
C.
Back
,
G.
Rossi
,
M.
Taguchi
,
H.
Daimon
,
G.
Van Der Laan
,
G.
Panaccione
Diamond Proposal Number(s):
[11322]
Abstract: In the rapidly growing field of spintronics, simultaneous control of electronic and magneticproperties is essential, and the perspective of building novel phases is directly linked to the control of tuning parameters, for example, thickness and doping. Looking at the relevanteffects in interface-driven spintronics, the reduced symmetry at a surface and interface corresponds to a severe modification of the overlap of electron orbitals, that is, to a change of electron hybridization. Here we report a chemically and magnetically sensitive depth-dependent analysis of two paradigmatic systems, namely La1xSrxMnO3 and (Ga,Mn)As. Supported by cluster calculations, we find a crossover between surface and bulk in the electron hybridization/correlation and we identify a spectroscopic fingerprint of bulk metallic character and ferromagnetism versus depth. The critical thickness and the gradient of hybridization are measured, setting an intrinsic limit of 3 and 10 unit cells from the surface,respectively, for (Ga,Mn)As and La1xSrxMnO3, for fully restoring bulk properties.
|
Jul 2017
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