arXiv subjects

Vincent Polewczyk

Publications and source records attributed to Vincent Polewczyk.

18 recordsLinked to original sources

arXiv2026

High temperature ferromagnetism in epitaxial monolayers of Co-doped Fe5GeTe2

Magnetic van der Waals materials have mainly been investigated in their bulk form or as few-layers flakes. Due to the challenges in producing atomically thin films, only a few have been isolated as monolayers, which typically exhibit long-range magnetic order below 150 K. In this work, we use molecular beam epitaxy to synthesize Co-doped Fe5GeTe2, achieving precise control over both thickness and composition. We demonstrate ferromagnetism well above room temperature in multilayer samples and present clear evidence of ferromagnetic ordering in monolayers up to $\sim$200 K. The changes in Curie temperature and magnetic anisotropy with composition exhibit similar trends in both monolayers and thicker films, indicating that the magnetic properties are primarily governed by intralayer magnetic interactions. Through element-specific X-ray magnetic circular dichroism and density functional theory, we identify the substitution site of Co dopants and reveal the mechanism behind the Curie temperature enhancement induced by Co doping. Our findings suggest that, despite their weak magnetic moment, Co dopants strengthen the magnetic moments on neighboring Fe atoms and enhance the intralayer ferromagnetic exchange interactions.

cond-mat.mtrl-sci↗

arXiv2026

Rashba engineering at van der Waals interfaces

Two-dimensional transition metal dichalcogenide (TMD) interfaces offer a versatile platform for studying emergent quantum phenomena and enabling novel device functionalities. When distinct TMD monolayers are stacked vertically or laterally stitched, their interfaces can exhibit unique electronic band alignments, giving rise to long-lived interlayer excitons, charge transfer effects, and moir\'e superlattices with correlated states. Here, we demonstrate that the interface between a large variety of two different epitaxially grown TMD monolayers controls the intensity and sign of the Rashba spin splitting, which is probed using THz spintronic emission. Optimized TMD heterobilayers, such as HfSe$_2$/PtSe$_2$, show enhanced THz emission that surpass the spin-to-charge conversion efficiency of bulk TMDs, confirming the presence of Rashba states with large spin splitting at the interface. By combining spin- and angle-resolved photoemission spectroscopy with density functional theory, we reveal that the electronic hybridization between the two different TMD monolayers gives rise to extended in-gap states with strong Rashba spin-orbit coupling. The choice of TMD layers enables to engineer the sign and strength of spin-to-charge conversion in van der Waals heterobilayers opening up perspectives to build efficient and tunable THz spintronic emitters.

cond-mat.mes-hall↗

arXiv2026

Synthesis and Transfer of Freestanding Strain-Engineered Vertically Aligned Nanocomposite Thin Films

The recent development of freestanding oxide thin films opens up exciting opportunities for the design of novel heterostructures with enhanced functionalities. Here, we explore the fabrication of membranes consisting of dense arrays of ultrathin CoxNi1-x nanowires epitaxially embedded in a SrTiO3 matrix. Through combined x-ray absorption spectroscopy, x-ray resonant magnetic scattering, x-ray diffraction and magnetooptical experiments, we show how a SrVO3-mediated lift-off process can be used to create and transfer these membranes while simultaneously preserving the structural and chemical integrity of the self-assembled, metallic CoxNi1-x nanopillars. With this approach, the large axial deformation of the embedded nanostructures is kept intact and, as a direct consequence, the magnetic properties of the nano-composite thin films remain largely unaltered after substrate removal. Our findings thus highlight a novel route for the synthesis of freestanding, strain-engineered vertically aligned heterostructures and pave the way for their future integration into spintronic and optomagnetic devices.

cond-mat.mtrl-sci↗

arXiv2025

Light-induced photomechanical patterning of ferroelectric polarization

Tailoring at will polar textures in ferroelectrics is critical for the development of nanoscale electronics and functional oxide technologies. Freestanding ferroelectric membranes have enabled studies of strain-induced polarization responses, but the control over membrane shape and local polarization typically remains limited to spontaneous buckling or uniaxial mechanical deformations. In this work, we employ a versatile photosensitive-polymer patterning approach to impose programmable bending strain profiles in ferroelectric membranes. Using BaTiO3 as a model system, we demonstrate deterministic 90{\deg} polarization rotation driven by engineered in-plane strain, and 180{\deg} polarization reversal arising from flexoelectric coupling through a controlled strain gradient. These results establish this programmable bending as a powerful approach to investigate strain-dependent domain structures, leverage flexoelectric effects, and engineer custom ferroelectric landscapes across a wide range of oxide membranes.

cond-mat.mtrl-sci↗

arXiv2025

Resonant Self-Diffraction of Femtosecond Extreme Ultraviolet Pulses in Cobalt

Self-diffraction is a non-collinear four-wave mixing technique well-known in optics. We explore self-diffraction in the extreme ultraviolet (EUV) range, taking advantage of intense femtosecond EUV pulses produced by a free electron laser. Two pulses are crossed in a thin cobalt film and their interference results in a spatially periodic electronic excitation. The diffraction of one of the same pulses by the associated refractive index modulation is measured as a function of the EUV wavelength. A sharp peak in the self-diffraction efficiency is observed at the M$_{2,3}$ absorption edge of cobalt at 59 eV and a fine structure is found above the edge. The results are compared with a theoretical model assuming that the excitation results in an increase of the electronic temperature. EUV self-diffraction offers a potentially useful spectroscopy tool and will be instrumental in studying coherent effects in the EUV range.

physics.optics↗

arXiv2025

Robust spin splitting and fermiology in a layered altermagnet

Altermagnetism defies conventional classifications of collinear magnetic phases, standing apart from ferromagnetism and antiferromagnetism with its unique combination of spin-dependent symmetries, net-zero magnetization, and anomalous Hall transport. Although altermagnetic states have been realized experimentally, their integration into functional devices has been hindered by the structural rigidity and poor tunability of existing materials. First, through cobalt intercalation of the superconducting 2H-NbSe$_2$ polymorph, we induce and stabilize a robust altermagnetic phase and using both theory and experiment, we directly observe the lifting of Kramers degeneracy. Additionally, we present spectroscopic insight into a previously hinted low-temperature phase, and provide evidence of its electronic origin. While shedding light on overlooked aspects of altermagnetism, these findings open pathways to spin-based technologies and lay a foundation for advancing the emerging field of altertronics.

cond-mat.str-el↗

arXiv2025

Anomalous spin-optical helical effect in Ti-based kagome metal

The kagome lattice stands as a rich platform for hosting a wide array of correlated quantum phenomena, ranging from charge density waves and superconductivity to electron nematicity and loop current states. Direct detection of loop currents in kagome systems has remained a formidable challenge due to their intricate spatial arrangements and the weak magnetic field signatures they produce. This has left their existence and underlying mechanisms a topic of intense debate. In this work, we uncover a hallmark reconcilable with loop currents: spin handedness-selective signals that surpass conventional dichroic, spin, and spin-dichroic responses. We observe this phenomenon in the kagome metal CsTi$_3$Bi$_5$ and we call it the anomalous spin-optical helical effect. This effect arises from the coupling of light' s helicity with spin-orbital electron correlations, providing a groundbreaking method to visualize loop currents in quantum materials. Our discovery not only enriches the debate surrounding loop currents but also paves the way for new strategies to exploit the electronic phases of quantum materials via light-matter interaction.

cond-mat.str-el↗

arXiv2024

Bilayer orthogonal ferromagnetism in CrTe$_2$-based van der Waals system

Systems with pronounced spin anisotropy play a pivotal role in advancing magnetization switching and spin-wave generation mechanisms, which are fundamental for spintronic technologies. Quasi-van der Waals ferromagnets, particularly Cr$_{1+\delta}$Te$_2$ compounds, represent seminal materials in this field, renowned for their delicate balance between frustrated layered geometries and magnetism. Despite extensive investigation, the precise nature of their magnetic ground state, typically described as a canted ferromagnet, remains contested, as does the mechanism governing spin reorientation under external magnetic fields and varying temperatures. In this work, we leverage a multimodal approach, integrating complementary techniques, to reveal that Cr$_{1+\delta}$Te$_2$ ($\delta = 0.25 - 0.50$) hosts a previously overlooked magnetic phase, which we term orthogonal-ferromagnetism. This single phase consists of alternating atomically sharp single layers of in-plane and out-of-plane ferromagnetic blocks, coupled via exchange interactions and as such, it differs significantly from crossed magnetism, which can be achieved exclusively by stacking multiple heterostructural elements together. Contrary to earlier reports suggesting a gradual spin reorientation in CrTe$_2$-based systems, we present definitive evidence of abrupt spin-flop-like transitions. This discovery, likely due to the improved crystallinity and lower defect density in our samples, repositions Cr$_{1+\delta}$Te$_2$ compounds as promising candidates for spintronic and orbitronic applications, opening new pathways for device engineering.

cond-mat.str-el↗

arXiv2024

Thermal treatment effects on PMN-0.4PT/Fe multiferroic heterostructures

Multiferroic heterostructures have gained in recent years a renewed role in spintronic applications due to their possibility in controlling the magnetic properties via interfacial coupling by exploiting the ferroelectric response to various external stimuli. Whereas the main mechanisms ruling the converse magnetoelectric coupling are considered as established, the research on how to optimize the ferroelectric properties is an active field. In particular the complex phase diagram of [Pb(Mg1/3Nb2/3)O3]-x[PbTiO3] (PMN-xPT) single crystals, that present relaxor ferroelectric and photovoltaic properties, deserves further investigation. For instance, crystalline quality and thermal stability of the ferroelectric domains in heterostructures need assessment. Here we show how, by thermal annealing over the ferroelectric Curie temperature and then cooling PMN-0.4PT/Fe heterostructures in inert atmosphere the domain population is significantly modified, evolving from a highly disordered, mostly out-of-plane domain population, to improved crystallinity and prevalent in-plane oriented domains. Upon further annealing, the domain population switches back to prevalent out-of-plane orientation suggesting that intermediate annealing steps can freeze PMN-0.4PT domain population in a metastable configuration. The structural analysis was carried out by combining micro-Raman and X-ray diffraction (XRD) measurements. In the three states the magnetic properties of interfacial Fe thin film are affected by the ferroelectric configurations as a consequence of changing interfacial strain, evolving from an isotropic behavior to an anisotropic one and back.

cond-mat.mtrl-sci↗

arXiv2024

Uncovering the lowest thickness limit for room-temperature ferromagnetism of Cr$_{1.6}$Te$_{2}$

Metallic ferromagnetic transition metal dichalcogenides have emerged as important building blocks for scalable magnonics and memory applications. Downscaling such systems to the ultra-thin limit is critical to integrate them into technology. Here, we achieved layer-by-layer control over the transition metal dichalcogenide Cr$_{1.6}$Te$_{2}$ by using pulsed laser deposition, and we uncovered the minimum critical thickness above which room temperature magnetic order is maintained. The electronic and magnetic structure is explored experimentally and theoretically and it is shown that the films exhibit strong in-plane magnetic anisotropy as a consequence of large spin-orbit effects. Our study elucidates both magnetic and electronic properties of Cr$_{1.6}$Te$_{2}$, and corroborates the importance of intercalation to tune the magnetic properties of nanoscale materials architectures.

cond-mat.mtrl-sci↗

arXiv2024

Signatures of a surface spin-orbital chiral metal

The relation between crystal symmetries, electron correlations, and electronic structure steers the formation of a large array of unconventional phases of matter, including magneto-electric loop currents and chiral magnetism. Detection of such hidden orders is a major goal in condensed matter physics. However, to date, nonstandard forms of magnetism with chiral electronic ordering have been experimentally elusive. Here, we develop a theory for symmetry-broken chiral ground states and propose a methodology based on circularly polarized spin-selective angular-resolved photoelectron spectroscopy to probe them. We exploit the archetypal quantum material Sr2RuO4 and reveal spectroscopic signatures which, even though subtle, may be reconciled with the formation of spin-orbital chiral currents at the material surface. As we shed light on these chiral regimes, our findings pave the way for a deeper understanding of ordering phenomena and unconventional magnetism.

cond-mat.str-el↗

arXiv2023

The electronic structure of intertwined kagome, honeycomb, and triangular sublattices of the intermetallics MCo$_2$Al$_9$

Intermetallics are an important playground to stabilize a large variety of physical phenomena, arising from their complex crystal structure. The ease of their chemical tuneabilty makes them suitable platforms to realize targeted electronic properties starting from the symmetries hidden in their unit cell. Here, we investigate the family of the recently discovered intermetallics MCo$_2$Al$_9$ (M: Sr, Ba) and we unveil their electronic structure for the first time. By using angle-resolved photoelectron spectroscopy and density functional theory calculations, we discover the existence of Dirac-like dispersions as ubiquitous features in this family, coming from the hidden kagome and honeycomb symmetries embedded in the unit cell. Finally, from calculations, we expect that the spin-orbit coupling is responsible for opening energy gaps in the electronic structure spectrum, which also affects the majority of the observed Dirac-like states. Our study constitutes the first experimental observation of the electronic structure of MCo$_2$Al$_9$ and proposes these systems as hosts of Dirac-like physics with intrinsic spin-orbit coupling. The latter effect suggests MCo$_2$Al$_9$ as a future platform for investigating the emergence of non-trivial topology.

cond-mat.str-el↗

arXiv2023

Flat band separation and robust spin-Berry curvature in bilayer kagome metals

Kagome materials have emerged as a setting for emergent electronic phenomena that encompass different aspects of symmetry and topology. It is debated whether the XV$_6$Sn$_6$ kagome family (where X is a rare earth element), a recently discovered family of bilayer kagome metals, hosts a topologically non-trivial ground state resulting from the opening of spin-orbit coupling gaps. These states would carry a finite spin-Berry curvature, and topological surface states. Here, we investigate the spin and electronic structure of the XV$_6$Sn$_6$ kagome family. We obtain evidence for a finite spin-Berry curvature contribution at the center of the Brillouin zone, where the nearly flat band detaches from the dispersing Dirac band because of spin-orbit coupling. In addition, the spin-Berry curvature is further investigated in the charge density wave regime of ScV$_6$Sn$_6$, and it is found to be robust against the onset of the temperature-driven ordered phase. Utilizing the sensitivity of angle resolved photoemission spectroscopy to the spin and orbital angular momentum, our work unveils the spin-Berry curvature of topological kagome metals, and helps to define its spectroscopic fingerprint.

cond-mat.str-el↗

arXiv2023

Covalency, correlations, and inter-layer interactions governing the magnetic and electronic structure of Mn$_3$Si$_2$Te$_6$

Mn$_3$Si$_2$Te$_6$ is a rare example of a layered ferrimagnet. It has recently been shown to host a colossal angular magnetoresistance as the spin orientation is rotated from the in- to out-of-plane direction, proposed to be underpinned by a topological nodal-line degeneracy in its electronic structure. Nonetheless, the origins of its ferrimagnetic structure remain controversial, while its experimental electronic structure, and the role of correlations in shaping this, are little explored to date. Here, we combine x-ray and photoemission-based spectroscopies with first-principles calculations, to probe the elemental-selective electronic structure and magnetic order in Mn$_3$Si$_2$Te$_6$. Through these, we identify a marked Mn-Te hybridisation, which weakens the electronic correlations and enhances the magnetic anisotropy. We demonstrate how this strengthens the magnetic frustration in Mn$_3$Si$_2$Te$_6$, which is key to stabilising its ferrimagnetic order, and find a crucial role of both exchange interactions extending beyond nearest-neighbours and anti-symmetric exchange in dictating its ordering temperature. Together, our results demonstrate a powerful methodology of using experimental electronic structure probes to constrain the parameter space for first-principles calculations of magnetic materials, and through this approach, reveal a pivotal role played by covalency in stabilising the ferrimagnetic order in Mn$_3$Si$_2$Te$_6$.

cond-mat.mtrl-sci↗

arXiv2023

Dynamics and Resilience of the Charge Density Wave in a bilayer kagome metal

Long-range electronic order descending from a metallic parent state constitutes a rich playground to study the intricate interplay of structural and electronic degrees of freedom. With dispersive and correlation features as multifold as topological Dirac-like itinerant states, van-Hove singularities, correlated flat bands, and magnetic transitions at low temperature, kagome metals are located in the most interesting regime where both phonon and electronically mediated couplings are significant. Several of these systems undergo a charge density wave (CDW) transition, and the van-Hove singularities, which are intrinsic to the kagome tiling, have been conjectured to play a key role in mediating such an instability. However, to date, the origin and the main driving force behind this charge order is elusive. Here, we use the topological bilayer kagome metal ScV6Sn6 as a platform to investigate this puzzling problem, since it features both kagome-derived nested Fermi surface and van-Hove singularities near the Fermi level, and a CDW phase that affects the susceptibility, the neutron scattering, and the specific heat, similarly to the siblings AV3Sb5 (A = K, Rb, Cs) and FeGe. We report on our findings from high-resolution angle-resolved photoemission, density functional theory, and time-resolved optical spectroscopy to unveil the dynamics of its CDW phase. We identify the structural degrees of freedom to play a fundamental role in the stabilization of charge order. Along with a comprehensive analysis of the subdominant impact from electronic correlations, we find ScV6Sn6 to feature an instance of charge density wave order that predominantly originates from phonons. As we shed light on the emergent phonon profile in the low-temperature ordered regime, our findings pave the way for a deeper understanding of ordering phenomena in all CDW kagome metals.

cond-mat.str-el↗

arXiv2022

Disentangling structural and electronic properties in V$_{2}$O$_{3}$ thin films: a genuine non-symmetry breaking Mott transition

Phase transitions are key in determining and controlling the quantum properties of correlated materials. Here, by using the powerful combination of precise material synthesis and angle resolved photoelectron spectroscopy, we show evidence for a genuine Mott transition undressed of any symmetry breaking side effects in the thin-films of V$_{2}$O$_{3}$. In particular, and in sharp contrast with the bulk V$_{2}$O$_{3}$ crystals, we unveil the purely electronic dynamics approaching the metal-insulator transition, disentangled from the structural transformation that is prevented by the residual substrate-induced strain. On approaching the transition, the spectral signal evolves surprisingly slowly over a wide temperature range, the Fermi wave-vector does not change, and the critical temperature appears to be much lower than the one reported for the bulk. Our findings are on one side fundamental in demonstrating the universal benchmarks of a genuine non-symmetry breaking Mott transition, extendable to a large array of correlated quantum systems and, on the other, given that the fatal structural breakdown is avoided, they hold promise of exploiting the metal-insulator transition by implementing V$_{2}$O$_{3}$ thin films in devices.

cond-mat.str-el↗

arXiv2020

Magnetic correlations in polycrystalline $\mathrm{Tb_{0.15}Co_{0.85}}$

We investigated a polycrystalline sample of the ferrimagnetic compound $\mathrm{Tb_{0.15}Co_{0.85}}$ by magnetometry and small-angle neutron scattering (SANS). The magnetization curve at 300 K is characteristic for soft ferrimagnets but at 5 K the hysteresis indicates the existence of magnetic domains. The magnetic SANS signal suggests that at 300 K the Tb and Co moments are correlated over large volumes within the micrometer-sized grains with correlation lengths > 100 nm. At 5 K, however, the magnetic SANS analysis reveals a reduced correlation length of around 4.5 nm, which indicates the formation of narrow magnetic domains within the ferrimagnet with one dimension being in the nm range. We attribute the observed changes of the domain structure to the temperature-dependence of the magnetic properties of the Tb sublattice.

cond-mat.mes-hall↗

arXiv2019

Stoichiometric Lithium Niobate Crystals: Towards Identifiable Wireless Surface Acoustic Wave Sensors Operable up to 600$^\circ$C

Wireless surface acoustic wave (SAW) sensors constitute a promising solution to some unsolved industrial sensing issues taking place at high temperatures. Currently, this technology enables wireless measurements up to 600-700$^\circ$C at best. However, the applicability of such sensors remains incomplete since they do not allow identification above 400$^\circ$C. The latter would require the use of a piezoelectric substrate providing a large electromechanical coupling coefficient K 2 , while being stable at high temperature. In this letter, we investigate the potentiality of stoichiometric lithium niobate (sLN) crystals for such purpose. Raman spectroscopy and X-ray diffraction attest that sLN crystals withstand high temperatures up to 800$^\circ$C, at least for several days. In situ measurements of sLN-based SAW resonators conducted up to 600$^\circ$C show that the K 2 of these crystals remains high and stable throughout the whole experiment, which is very promising for the future achievement of identifiable wireless high-temperature SAW sensors.

physics.app-ph↗