arXiv subjects

Victor Porée

Publications and source records attributed to Victor Porée.

11 recordsLinked to original sources

arXiv2026

Emergent 3D Fermiology and Magnetism in an Intercalated Van der Waals System

Intercalation of magnetic atoms into van der Waals materials provides a versatile platform for tailoring unconventional magnetic properties. However, its impact on electronic dimensionality and exchange mechanisms remains poorly understood. Using Fe-intercalated TaS$_2$ as a model system, we combine X-ray absorption and resonant inelastic scattering with angle-resolved photoemission and first-principles calculations to reveal that intercalation reshapes the host electronic structure. We identify a spin-polarized intercalant-host hybridized band with pronounced out-of-plane dispersion crossing the Fermi level, providing an itinerant channel for interlayer magnetic exchange. This mechanism explains the breakdown of a purely atomic picture and establishes a direct link between lattice geometry, electronic dispersion, and magnetic order. Our findings demonstrate that intercalant-induced itinerancy enables tunable interlayer coupling in otherwise layered magnets, offering a general microscopic framework for engineering magnetic dimensionality in a broad class of intercalated vdW materials.

cond-mat.mtrl-sci↗

arXiv2025

Dipolar-octupolar correlations and hierarchy of exchange interactions in Ce$_2$Hf$_2$O$_7$

High-resolution neutron spectroscopy on Ce$_2$Hf$_2$O$_7$ reveals a correlated state characterized by distinct dipolar scattering signals -- quasi-elastic and inelastic contributions consistent with `photon' and `spinon' excitations in quantum spin ice. These signals coexist with weak octupolar scattering. Fits of thermodynamic data using numerical methods indicate a dominant octupolar exchange, $J_{x}$ or $J_{y}$, with substantial dipolar $J_{z}$ and minute dipole-octupole $J_{xz}$ couplings. The $J_{xz}$ value is corroborated by an independent fit of the neutron scattering amplitude balance between dipolar and octupolar `photon' contributions, highlighting its importance to understand neutron scattering results in this family. Ce$_2$Hf$_2$O$_7$ enriches the landscape of dipole-octupole pyrochlore physics, and reveals a `quantum multipolar liquid' where hybrid correlations involve multiple terms in moment series expansion, opening questions on their intertwining and hierarchy in quantum phases.

cond-mat.str-el↗

arXiv2025

Thermodynamics of the dipole-octupole pyrochlore magnet Ce$_2$Hf$_2$O$_{7}$ in applied magnetic fields

The recently discovered dipole-octupole pyrochlore magnet Ce$_2$Hf$_2$O$_7$ is a promising three-dimensional quantum spin liquid candidate which shows no signs of ordering at low temperature. The low energy effective pseudospin-1/2 description in a magnetic field is characterized by the XYZ Hamiltonian and a Zeeman term where the dipolar local $z$-component of the pseudospin couples to the local $z$-component of the applied magnetic field, while the local $x$- and $y$-components of the pseudospin remain decoupled as a consequence of their octupolar character. Using effective Hamiltonian parameters determined in V. Poree et al., arXiv:2305.08261 (2023), remarkable experimental features can be reproduced, as for instance the specific heat and magnetization data as well as the continuum of states seen in neutron scattering. Here we investigate the thermodynamic response to magnetic fields applied along the global [110] direction using specific heat measurements and fits using numerical methods, and solve the corresponding magnetic structure using neutron diffraction. Specific heat data in moderate fields are reproduced well, however, at high fields the agreement is not satisfactory. We especially observe a two-step release of entropy, a finding that demands a review of both theory and experiment. We address it within the framework of three possible scenarios, including an analysis of the crystal field Hamiltonian not restricted to the two-dimensional single-ion doublet subspace. We conclusively rule out two of these scenarios and find qualitative agreement with a simple model of field misalignment with respect to the crystalline direction. We discuss the implications of our findings for [111] applied fields and for future experiments on Ce$_2$Hf$_2$O$_7$ and its sister compounds.

cond-mat.str-el↗

arXiv2025

Direct measurement of the longitudinal exciton dispersion in hBN by resonant inelastic x-ray scattering

We report resonant inelastic X-ray scattering (RIXS) measurements on the prototypical hexagonal boron nitride hBN layered compound. The RIXS results at the B and N K edges have been combined with electron energy loss spectroscopy (EELS) experiments and ab initio calculations within the framework of the Bethe-Salpeter equation of many-body perturbation theory. By means of this tight interplay of different spectroscopies, the lowest longitudinal exciton of hBN has been identified. Moreover, its qualitatively different dispersions along the $Γ$K and the $Γ$M directions of the Brillouin zone have been determined. Our study advocates soft X-ray RIXS and EELS to be a promising combination to investigate electronic excitations in materials.

cond-mat.mtrl-sci↗

arXiv2025

Resonant X-ray spectroscopies on Chromium $3\textit{d}$ orbitals in CrSBr

We investigate the Cr electronic structure and excitations in CrSBr, a layered magnetic semiconductor, using a combination of resonant x-ray spectroscopic techniques. X-ray absorption spectroscopy (XAS) and resonant inelastic x-ray scattering (RIXS) spectra collected at the Cr $L_{2,3}$ edges reveal significant linear dichroism, which arises from the distorted octahedral environment surrounding the Cr$^{3+}$ ions. The origin of the bright excitons observed in this compound is examined through a comparison of the d-d excitations identified in the RIXS spectra, the x-ray excited optical luminescence (XEOL) spectra, and previously reported optical spectroscopic and theoretical studies. To further understand these phenomena, we develop a multiplet model based on a crystal electric field (CEF) approach that accounts for the local environment of Cr ions. This model successfully reproduces several experimental features, while also suggesting strong hybridization effects between Cr $3\textit{d}$ orbitals and ligands that are not fully captured by the present framework. These findings advance our understanding of the electronic structure and excitonic behavior in CrSBr and provide a foundation for future $\textit{in-situ}$ and $\textit{operando}$ studies of CrSBr-based devices for spintronic and optoelectronic applications.

cond-mat.mtrl-sci↗

arXiv2024

Fractional matter coupled to the emergent gauge field in a quantum spin ice

Electronic spins can form long-range entangled phases of condensed matter named quantum spin liquids. Their existence is conceptualized in models of two- or three-dimensional frustrated magnets that evade symmetry-breaking order down to zero temperature. Quantum spin ice (QSI) is a theoretically well-established example described by an emergent quantum electrodynamics, with excitations behaving like photon and matter quasiparticles. The latter are fractionally charged and equivalent to the `spinons' emerging from coherent phases of singlets in one dimension, where clear experimental proofs of fractionalization exist. However, in frustrated magnets it remains difficult to establish consensual evidence for quantum spin liquid ground states and their fractional excitations. Here, we use backscattering neutron spectroscopy to achieve extremely high resolution of the time-dependent magnetic response of the candidate QSI material Ce$_2$Sn$_2$O$_7$. We find a gapped spectrum featuring a threshold and peaks that match theories for pair production and propagation of fractional matter excitations (spinons) strongly coupled to a background gauge field. The multiple peaks are a specific signature of the $π$-flux phase of QSI, providing spectroscopic evidence for fractionalization in a three-dimensional quantum spin liquid.

cond-mat.str-el↗

arXiv2024

YBa$_{1-x}$Sr$_{x}$CuFeO$_{5}$ layered perovskites: exploring the magnetic order beyond the paramagnetic-collinear-spiral triple point

Layered perovskites of general formula AA'CuFeO$_5$ are one of the few examples of cycloidal spiral magnets where the ordering temperatures $T_{spiral}$ can be tuned far beyond room temperature by introducing modest amounts of Cu/Fe chemical disorder in the crystal structure. This rare property makes these materials prominent candidates to host multiferroicity and magnetoelectric coupling at room temperature. Moreover, it has been proposed that the highest $T_{spiral}$ value that can be reached in this structural family ($\sim$ 400 K) corresponds to a paramagnetic-collinear-spiral triple point with potential to show exotic physics. Since generating high amounts of Cu/Fe disorder is experimentally difficult, the phase diagram region beyond the triple point has been barely explored. To fill this gap we investigate here the YBa$_{1-x}$Sr$_{x}$CuFeO$_{5}$ solid solutions ($0 \leq x \leq 1$), where we replace Ba with Sr with the aim of enhancing the impact of the experimentally available Cu/Fe disorder. Using a combination of bulk magnetization, synchrotron X-ray and neutron powder diffraction we show that the spiral state is destabilized beyond a critical degree of Cu/Fe disorder, being replaced by a non-frustrated, fully antiferromagnetic state with propagation vector k$_{c2}$ = $(\frac{1}{2}, \frac{1}{2}, 0)$ and ordering temperature $T_{coll2}$ $\geq$ $T_{spiral}$, which is progressively stabilized beyond the triple point. Interestingly, $T_{spiral}$ and $T_{coll2}$ increase with $x$ at the same rate. This suggests a common, disorder-driven origin, consistent with theoretical predictions.

cond-mat.str-el↗

arXiv2023

Emergent electronic landscapes in a novel valence-ordered nickelate with tri-component nickel coordination

The metal-hydride-based topochemical reduction process has produced novel thermodynamically unstable phases across various transition metal oxide series with unusual crystal structures and non-trivial ground states. Here, by such an oxygen (de-) intercalation method we synthesis a novel samarium nickelate with ordered nickel valences associated with tri-component coordination configurations. This structure, with a formula of Sm$_{9}$Ni$_{9}$O$_{22}$ as revealed by four-dimensional scanning transmission electron microscopy, emerges from the intricate planes of {303}$_{\text{pc}}$ ordered apical oxygen vacancies. X-ray spectroscopy measurements and ab-initio calculations show the coexistence of square-planar, pyramidal and octahedral Ni sites with mono-, bi- and tri-valences. It leads to an intense orbital polarization, charge-ordering, and a ground state with a strong electron localization marked by the disappearance of ligand-hole configuration at low-temperature. This new nickelate compound provides another example of previously inaccessible materials enabled by topotactic transformations and presents a unique platform where mixed Ni valence can give rise to exotic phenomena.

cond-mat.mtrl-sci↗

arXiv2022

Crystal-field states and defect levels in candidate quantum spin ice Ce$_{2}$Hf$_{2}$O$_{7}$

We report the synthesis of powder and single-crystal samples of the cerium pyrohafnate and their characterization using neutron diffraction, thermogravimetry and X-ray absorption spectroscopy. We evaluate the amount of non-magnetic Ce$^{4+}$ defects and use this result to interpret the spectrum of crystal-electric field transitions observed using inelastic neutron scattering. The analysis of these single-ion transitions indicates the dipole-octupole nature of the ground state doublet and a significant degree of spin-lattice coupling. The single-ion properties calculated from the crystal-electric field parameters obtained spectroscopically are in good agreement with bulk magnetic susceptibility data down to about 1 K. Below this temperature, the behavior of the magnetic susceptibility indicates a correlated regime without showing any sign of magnetic long-range order or freezing down to 0.08 K. We conclude that Ce$_2$Hf$_2$O$_{7}$ is another candidate to investigate exotic correlated states of quantum matter such as the octupolar quantum spin ice recently argued to exist in the isostructural compounds Ce$_2$Sn$_2$O$_7$ and Ce$_2$Zr$_2$O$_7$.

cond-mat.str-el↗

arXiv2020

Neutron scattering by magnetic octupoles of a quantum liquid

Neutron scattering is a powerful tool to study magnetic structures and dynamics, benefiting from a precisely established theoretical framework. The neutron dipole moment interacts with electrons in materials via their magnetic field, which can have spin and orbital origins. Yet in most experimentally studied cases the individual degrees of freedom are well described within the dipole approximation, sometimes accompanied by further terms of a multipolar expansion that usually act as minor corrections to the dipole form factor. Here we report a unique example of neutrons diffracted mainly by magnetic octupoles. This unusual situation arises in a quantum spin ice where the electronic wavefunction becomes essentially octupolar under the effect of correlations. The discovery of such a new type of quantum spin liquid that comes with a specific experimental signature in neutron scattering is remarkable, because these topical states of matter are notoriously difficult to detect.

cond-mat.str-el↗

arXiv2019

A quantum liquid of magnetic octupoles on the pyrochlore lattice

Spin liquids are highly correlated yet disordered states formed by the entanglement of magnetic dipoles$^1$. Theories typically define such states using gauge fields and deconfined quasiparticle excitations that emerge from a simple rule governing the local ground state of a frustrated magnet. For example, the '2-in-2-out' ice rule for dipole moments on a tetrahedron can lead to a quantum spin ice in rare-earth pyrochlores - a state described by a lattice gauge theory of quantum electrodynamics$^{2-4}$. However, f-electron ions often carry multipole degrees of freedom of higher rank than dipoles, leading to intriguing behaviours and 'hidden' orders$^{5-6}$. Here we show that the correlated ground state of a Ce$^{3+}$-based pyrochlore, Ce$_2$Sn$_2$O$_7$, is a quantum liquid of magnetic octupoles. Our neutron scattering results are consistent with the formation of a fluid-like state of matter, but the intensity distribution is weighted to larger scattering vectors, which indicates that the correlated degrees of freedom have a more complex magnetization density than that typical of magnetic dipoles in a spin liquid. The temperature evolution of the bulk properties in the correlated regime below 1 Kelvin is well reproduced using a model of dipole-octupole doublets on a pyrochlore lattice$^{7-8}$. The nature and strength of the octupole-octupole couplings, together with the existence of a continuum of excitations attributed to spinons, provides further evidence for a quantum ice of octupoles governed by a '2-plus-2-minus' rule. Our work identifies Ce$_2$Sn$_2$O$_7$ as a unique example of a material where frustrated multipoles form a 'hidden' topological order, thus generalizing observations on quantum spin liquids to multipolar phases that can support novel types of emergent fields and excitations.

cond-mat.str-el↗