arXiv subjects

Sylvain Petit

Publications and source records attributed to Sylvain Petit.

At least 19 recordsLinked to original sources

arXiv2026

Topological band structure of excitons in octochlore KTb$_{3}$F$_{10}$: an analog of the Luttinger Semimetal

Understanding the symmetry and topology of band structures in crystalline solids has been among the defining themes of a generation of condensed matter physicists, with implications across many different platforms including electronic bands, photonic crystals, phonons and magnetic excitations. In the latter systems, there is usually magnetic long-range order and time reversal symmetry breaking. Here we further enrich the possible band structures available to magnetic systems by examining dispersive crystal field excitations above a ground state that is a simple product of singlets. In these systems, there is an interplay of magnetic interactions and band topology with both crystal and time reversal symmetries. Using high-resolution neutron spectroscopy we reveal the dispersion relations of bosonic excitons in KTb$_{3}$F$_{10}$, an experimental realization of the octochlore lattice. We show that there are pinch point features in the scattering intensity. The dominant coupling in this system is the long-range magnetostatic dipolar interaction, whose singularity at the zone center is passed onto the scattering intensity. However, the pinch points survive when the range of the dipoles is truncated to finite shell number in the form of a three-band quadratic band touching protected by cubic symmetry. This model, which is related to the Luttinger semi-metal, provides a general long wavelength model for the emergence of pinch point scattering intensity encompassing also the true long-range dipolar model.

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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.

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arXiv2025

Altermagnetism revealed by polarized neutrons in MnF$_2$

Motivated by possible spintronics applications in antiferromagnets, it was recently observed that symmetry admits magnets that combine attractive features of both ferromagnets and antiferromagnets. These systems, dubbed altermagnets, have been the subject of intense study with direct spectroscopic evidence, from ARPES and RIXS, techniques reported in a handful of materials in the last year. Inelastic neutron scattering (INS) is one of the most powerful direct probes of magnetism and has recently been used to witness a splitting of magnon bands in MnTe that is compatible with altermagnetism although the nature and origin of the splitting remain to be fully characterized. However, the full power of neutron scattering for such systems comes from using polarized neutrons to measure the chirality of the magnon bands. Such a measurement provides a direct characterization of altermagnetism directly from the spin wave excitations. In this article, we present results on MnF$_2$ once thought to be an archetypal antiferromagnet. We present a polarized INS data that demonstrate the material is, in fact, altermagnetic. It had long been realized that the magnon bands in this material should have a weak splitting coming from the long-range dipolar coupling. Our data is the first to visualize this splitting directly. While the dipolar splitting on its own is not altermagnetic, using a domain biased sample, the data reveals a nonzero chirality in the neutron scattering cross section that reverses sign between the two magnon modes. It is this feature that clearly demonstrates altermagnetism in MnF$_2$. This finding highlights the potential for polarized INS to characterize altermagnets not least through its exquisite sensitivity to fine-structure in the magnon spectrum.

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arXiv2025

Geometrically Frustrated Quadrupoles on the Pyrochlore Lattice and Generalized Spin Liquids

As an instance of geometrical frustration with non-magnetic degrees of freedom, we explore the physics of local spin $S\geq 1$ moments on the pyrochlore lattice that interact via pure quadrupolar couplings. In the presence of spin-orbit coupling, there are nine allowed couplings between nearest neighbor quadrupoles. We determine the semi-classical phases and survey the phase diagram of the model. One may view the Hamiltonian as being composed of two copies of the well-studied dipolar model with couplings between the copies, and we find that each easy-plane dipolar phase has two quadrupolar counterparts. As geometrical frustration is important over broad swathes of the parameter space, there are many classical quadrupolar liquids and regions with order-by-disorder selection of discrete states. Order-by-disorder with quadrupoles admits cubic terms in the Landau theory whose effects appear in Monte Carlo simulations and flavor wave calculations for fixed spin $S$. We showcase a number of examples of quadrupolar spin liquids, including one realizing a rank-3 symmetric tensor gauge theory exhibiting 6-fold pinch point singularities. We discuss remarkable differences between the quadrupolar physics of different spin quantum number. We also discuss connections to the non-Kramers rare earth pyrochlore materials.

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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.

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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.

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arXiv2024

Impact of disorder in Nd-based pyrochlore magnets

We study the stability of the antiferromagnetic all-in--all-out state observed in dipolar-octupolar pyrochlores that have neodymium as the magnetic species. Different types of disorder are considered, either affecting the immediate environment of the Nd$^{3+}$ ion, or substituting it with a non-magnetic ion. Starting from the well studied Nd$_2$Zr$_2$O$_7$ compound, Ti substitution on the Zr site and dilution on the Nd magnetic site with La substitution are investigated. The recently discovered entropy stabilized compound NdMox, which exhibits a high degree of disorder on the non magnetic site is also studied. Using a range of experimental techniques, especially very low-temperature magnetization and neutron scattering, we show that the all-in--all-out state is very robust and withstands substitutional disorder up to large rates. From these measurements, we estimate the Hamiltonian parameters and discuss their evolution in the framework of the phase diagram of dipolar-octupolar pyrochlore magnets.

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arXiv2023

Phase transitions and spin dynamics of the quasi-one dimensional Ising-like antiferromagnet BaCo$_{2}$V$_{2}$O$_{8}$ in a longitudinal magnetic field

By combining inelastic neutron scattering and numerical simulations, we study the quasi-one dimensional Ising-like quantum antiferromagnet BaCo$_{2}$V$_{2}$O$_{8}$ in a longitudinal magnetic field applied along the magnetic anisotropy axis, which is also the chain direction. The external field closes the excitation gap due to the magnetic anisotropy, inducing a transition from the Néel ordered state to an incommensurate longitudinal spin density wave phase. If the field is increased further, another transition into a transverse antiferromagnetic phase takes place at 9 T due to the competition between longitudinal and transverse correlations. We numerically and experimentally show that the model of XXZ chains connected by a weak interchain interaction well reproduces this transition. We also calculate the dynamical susceptibility and demonstrate that it agrees quantitatively with inelastic neutron scattering measurements. In contrast to the abrupt change of magnetic ordering, the spectra do not change much at the transition at 9 T, and the spin dynamics can be described as a Tomonaga-Luttinger liquid. We also refine the modeling of BaCo$_{2}$V$_{2}$O$_{8}$ by including a four-site periodic term arising from the crystal structure which enables to account for an anomaly of the magnetic susceptibility appearing at 19 T as well as for the anticrossing observed in the inelastic neutron scattering spectra.

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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$_7$.

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arXiv2021

Solitonic excitations in the Ising anisotropic chain BaCo2V2O8 under large transverse magnetic field

We study the dynamics of the quasi-one-dimensional Ising-Heisenberg antiferromagnet BaCo2V2O8 under a transverse magnetic field. Combining inelastic neutron scattering experiments and theoretical analyses by field theories and numerical simulations, we mainly elucidate the structure of the spin excitation spectrum in the high field phase, appearing above the quantum phase transition point mu0Hc ~ 10 T. We find that it is characterized by collective solitonic excitations superimposed on a continuum. These solitons are strongly bound in pairs due to the effective staggered field induced by the nondiagonal g tensor of the compound, and are topologically different from the fractionalized spinons in the weak field region. The dynamical susceptibility numerically calculated with the infinite time-evolving block decimation method shows an excellent agreement with the measured spectra, which enables us to identify the dispersion branches with elementary excitations. The lowest energy dispersion has an incommensurate nature and has a local minimum at an irrational wave number due to the applied transverse field.

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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.

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arXiv2020

Successive incommensurate spin orderings and excitations in multiferroic SrMnGe2O6

Anisotropic multiferroic properties of SrMnGe2O6 pyroxene single crystals were systematically investigated by means of magnetization, heat capacity, pyroelectric current measurement and elastic and inelastic neutron scattering experiments. Single crystal neutron diffraction allows us to unambiguously reveal the presence of two incommensurate magnetic orderings: a non-polar amplitude-modulated collinear sinusoidal magnetic structure emerges at TN1=4.36(2)K followed by a polar elliptical cycloidal spin structure below TN2=4.05(2)K. Pyroelectric current measurements on single crystal confirm the appearance of a spontaneous polarization within the (ac) plane below TN2 associated with the latter magnetic symmetry through extended Dzyaloshinsky-Moriya mechanism. The magnetic phase diagram was calculated considering the three isotropic exchange couplings relevant in this system. The magnetic excitations spectra of SrMnGe2O6 measured by inelastic neutron scattering were successfully modeled using a set of exchange interactions consistent with this phase diagram.

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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.

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arXiv2019

Tomonaga-Luttinger liquid spin dynamics in the quasi-one dimensional Ising-like antiferromagnet BaCo$_2$V$_2$O$_8$

Combining inelastic neutron scattering and numerical simulations, we study the quasi-one dimensional Ising anisotropic quantum antiferromagnet \bacovo\ in a longitudinal magnetic field. This material shows a quantum phase transition from a Néel ordered phase at zero field to a longitudinal incommensurate spin density wave at a critical magnetic field of 3.8 T. Concomitantly the excitation gap almost closes and a fundamental reconfiguration of the spin dynamics occurs. These experimental results are well described by the universal Tomonaga-Luttinger liquid theory developed for interacting spinless fermions in one dimension. We especially observe the rise of mainly longitudinal excitations, a hallmark of the unconventional low-field regime in Ising-like quantum antiferromagnet chains.

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arXiv2019

Interacting chains of orbital polarons in "Colossal" magnetoresistive La1-xSrxMnO3 revealed by spin and lattice dynamics

The origin of the effect of colossal magneto-resistance (CMR) remains still unexplained. In this work we revisit the spin dynamics of the pseudo-cubic La1-xSrxMnO3 along the Mn-O-Mn bond direction at four x doping values (x < 0.5) and various temperatures and report a new lattice dynamics study at x0=0.2, representative of the optimal doping for CMR. We propose an interpretation of the spin dynamics in terms of orbital polarons. This picture is supported by the observation of a discrete magnetic energy spectrum Enmag (q) characteristic of the internal excitations of "orbital polarons" defined by Mn3+ neighbors surrounding a Mn4+ center with a hole. Because of its hopping, the hole mixes up dynamically all the possible orbital configurations of its surrounding Mn3+ sites with degenerate energies. The Enmag values indicate a lift of orbital degeneracy by phonon excitations. The number n varies with the spatial dimension D of the polaron and the q-range determines its size. At x=0.125 and x=0.3 the spectrum reveals 2D polarons coupled by exchange and 3D "free" polarons respectively, with sizes l=1.67a < 2a in all bond directions. At x0=0.2, the spin and the lattice dynamics provide evidence for chains of orbital polarons of size l=2a with a periodic distribution over ~ 3a and an interaction energy ~ 3 meV. At T < Tc the charges propagate together with the longitudinal acoustic phonons along the chains enhancing their ferromagnetic character. The phase separation between metallic and ferromagnetic chains in a non-metallic matrix may be crucial for CMR.

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arXiv2016

Helical bunching and symmetry lowering inducing multiferroicity in Fe langasites

The chiral Fe-based langasites represent model systems of triangle-based frustrated magnets with a strong potential for multiferroicity. We report neutron scattering measurements for the multichiral Ba3MFe3Si2O14 (M = Nb, Ta) langasites revealing new important features of the magnetic order of these systems: the bunching of the helical modulation along the c-axis and the in-plane distortion of the 120{\textdegree} Fe-spin arrangement. We discuss these subtle features in terms of the microscopic spin Hamiltonian, and provide the link to the magnetically-induced electric polarization observed in these systems. Thus, our findings put the multiferroicity of this attractive family of materials on solid ground.

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arXiv2015

Order by virtual crystal field fluctuations in pyrochlore XY antiferromagnets

Conclusive evidence of order by disorder is scarce in real materials. Perhaps one of the strongest cases presented has been for the pyrochlore XY antiferromagnet Er2Ti2O7, with the ground state selection proceeding by order by disorder induced through the effects of quantum fluctuations. This identification assumes the smallness of the effect of virtual crystal field fluctuations that could provide an alternative route to picking the ground state. Here we show that this order by virtual crystal field fluctuations is not only significant, but competitive with the effects of quantum fluctuations. Further, we argue that higher-multipolar interactions that are generically present in rare-earth magnets can dramatically enhance this effect. From a simplified bilinear-biquadratic model of these multipolar interactions, we show how the virtual crystal field fluctuations manifest in Er2Ti2O7 using a combination of strong coupling perturbation theory and the random phase approximation. We find that the experimentally observed psi2 state is indeed selected and the experimentally measured excitation gap can be reproduced when the bilinear and biquadratic couplings are comparable while maintaining agreement with the entire experimental spin-wave excitation spectrum. Finally, we comments on possible tests of this scenario and discuss implications for other order-by-disorder candidates in rare-earth magnets.

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arXiv2014

Magneto- to electro-active transmutation of spin waves in ErMnO3

The low energy dynamical properties of the multiferroic hexagonal perovskite ErMnO3 have been studied by inelastic neutron scattering as well as terahertz and far infrared spectroscopies on synchrotron source. From these complementary techniques, we have determined the magnon and crystal field spectra and identified a zone center magnon only excitable by the electric field of an electromagnetic wave. Using comparison with the isostructural YMnO3 compound and crystal field calculations, we propose that this dynamical magnetoelectric process is due to the hybridization of a magnon with an electro-active crystal field transition.

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