I09-Surface and Interface Structural Analysis
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Francesco
Offi
,
Francesco
Borgatti
,
Pasquale
Orgiani
,
Vincent
Polewczyk
,
Sandeep Kumar
Chaluvadi
,
Shyni
Punathum Chalil
,
Aleksandr
Petrov
,
Federico
Motti
,
Gian Marco
Pierantozzi
,
Giancarlo
Panaccione
,
Bogdan
Rutkowski
,
Paolo
Mengucci
,
Gianni
Barucca
,
Deepnarayan
Biswas
,
Tien-Lin
Lee
,
Emiliano
Marchetti
,
Alberto
Martinelli
,
Davide
Peddis
,
Gaspare
Varvaro
Diamond Proposal Number(s):
[32921]
Open Access
Abstract: Epitaxial heterostructures integrating thin Fe3O4 films hold great potential for spintronics, magnetoionics, and multifunctional device development. In this work, the morpho-structural and magnetic properties of all-spinel Fe3O4/MgCr2O4/Fe3O4 trilayers grown on a MgCr2O4 buffer-layer, exhibiting very close lattice matching, were investigated by using both surface and bulk sensitive techniques. The close lattice match between Fe3O4 and MgCr2O4 enables the growth of epitaxial heterostructures with magnetically decoupled Fe3O4 layers for spacer thicknesses ≥ 1.6 nm, while reducing the formation of antiphase boundaries. Despite localized interphase diffusion, which leads to the formation of a mixed Cr/Fe spinel oxide with magnetically polarized Cr ions at the Fe3O4/MgCr2O4 interfaces, the overall magnetic properties remain largely consistent with those of the individual Fe3O4 layers. This study sheds light on the magnetic interactions within Fe3O4 layers mediated by a MgCr2O4 spacer, and demonstrates the feasibility of the approach in preserving the properties of thin Fe3O4 films, in complex heterostructures, thus offering a promising pathway for designing advanced all-spinel oxide devices.
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May 2025
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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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I09-Surface and Interface Structural Analysis
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Curran
Kalha
,
Laura E.
Ratcliff
,
Giorgio
Colombi
,
Christoph
Schlueter
,
Bernard
Dam
,
Andrei
Gloskovskii
,
Tien-Lin
Lee
,
Pardeep K.
Thakur
,
Prajna
Bhatt
,
Yujiang
Zhu
,
Jürg
Osterwalder
,
Francesco
Offi
,
Giancarlo
Panaccione
,
Anna
Regoutz
Diamond Proposal Number(s):
[29451]
Open Access
Abstract: Metal hydrides are potential candidates for applications in hydrogen-related technologies, such as energy storage, hydrogen compression, and hydrogen sensing, to name just a few. However, understanding the electronic structure and chemical environment of hydrogen within them remains a key challenge. This work presents a new analytical pathway to explore these aspects in technologically relevant systems using hard x-ray photoelectron spectroscopy (HAXPES) on thin films of two prototypical metal dihydrides:
YH
2
−
δ
and
Ti
H
2
−
δ
. By taking advantage of the tunability of synchrotron radiation, a nondestructive depth profile of the chemical states is obtained using core-level spectra. Combining experimental valence-band (VB) spectra collected at varying photon energies with theoretical insights from density functional theory (DFT) calculations, a description of the bonding nature and the role of
d
versus
s
p
contributions to states near the Fermi energy are provided. Moreover, a reliable determination of the enthalpy of formation is proposed by using experimental values of the energy position of metal
s
-band features close to the Fermi energy in the HAXPES VB spectra.
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Nov 2023
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I05-ARPES
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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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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
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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
|
Chiara
Bigi
,
Zhenkun
Tang
,
Gian Marco
Pierantozzi
,
Pasquale
Orgiani
,
Pranab Kumar
Das
,
Jun
Fujii
,
Ivana
Vobornik
,
Tommaso
Pincelli
,
Alessandro
Troglia
,
Tien-Lin
Lee
,
Regina
Ciancio
,
Goran
Drazic
,
Alberto
Verdini
,
Anna
Regoutz
,
Phil D. C.
King
,
Deepnarayan
Biswas
,
Giorgio
Rossi
,
Giancarlo
Panaccione
,
Annabella
Selloni
Diamond Proposal Number(s):
[16041]
Abstract: Two-dimensional (2D) metallic states induced by oxygen vacancies (
V
O
s
) at oxide surfaces and interfaces provide opportunities for the development of advanced applications, but the ability to control the behavior of these states is still limited. We used angle resolved photoelectron spectroscopy combined with density-functional theory (DFT) to study the reactivity of
V
O
-induced states at the (001) surface of anatase
TiO
2
, where both 2D metallic and deeper lying in-gap states (IGs) are observed. The 2D and IG states exhibit remarkably different evolutions when the surface is exposed to molecular
O
2
: while IGs are almost completely quenched, the metallic states are only weakly affected. DFT calculations indeed show that the IGs originate from surface
V
O
s
and remain localized at the surface, where they can promptly react with
O
2
. In contrast, the metallic states originate from subsurface vacancies whose migration to the surface for recombination with
O
2
is kinetically hindered on anatase
TiO
2
(001), thus making them much less sensitive to oxygen dosing.
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Feb 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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