arXiv subjects

Virginie Simonet

Publications and source records attributed to Virginie Simonet.

At least 19 recordsLinked to original sources

arXiv2023

Lattice dynamics and spin excitations in the metal-organic framework [CH$_3$NH$_3$][Co(HCOO)$_3$]

In metal-organic-framework (MOF) perovskites, both magnetic and ferroelectric orderings can be readily realized by compounding spin and charge degrees of freedom. The hydrogen bonds that bridge the magnetic framework and organic molecules have long been thought of as a key in generating multiferroic properties. However, the underlying physical mechanisms remain unclear. Here, we combine neutron diffraction, quasielastic and inelastic neutron scattering, and THz spectroscopy techniques to thoroughly investigate the dynamical properties of the multiferroic MOF candidate [CH$_3$NH$_3$][Co(HCOO)$_3$] through its multiple phase transitions. The wide range of energy resolutions reachable by these techniques enables us to scrutinize the coupling between the molecules and the framework throughout the phase transitions and interrogate a possible magnetoelectric coupling. Our results also reveal a structural change around 220 K which may be associated with the activation of a nodding donkey mode of the methylammonium molecule due to the ordering of the CH$_3$ groups. Upon the occurrence of the modulated phase transition around 130 K, the methylammonium molecules undergo a freezing of its reorientational motions which is concomitant with a change of the lattice parameters and anomalies of collective lattice vibrations. No significant change has been however observed in the lattice dynamics around the magnetic ordering, which therefore indicates the absence of a substantial magneto-electric coupling in zero-field.

cond-mat.mtrl-sci↗

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.

cond-mat.str-el↗

arXiv2022

Vibronic collapse of ordered quadrupolar ice in the pyrochore magnet Tb$_{2+x}$Ti$_{2-x}$O$_{7+y}$

While the spin liquid state in the frustrated pyrochlore Tb$_{2+x}$Ti$_{2-x}$O$_{7+y}$ has been studied both experimentally and theoretically for more than two decades, no definite description of this unconventional state has been achieved. Using synchrotron based THz spectroscopy in combination with quantum numerical simulations, we highlight a significant link between two previously unrelated features: the existence of a quadrupolar order following an ice rule and the presence of strong magneto-elastic coupling in the form of hybridized Tb$^{3+}$ crystal-field and phonon modes. The magnitude of this so-called vibronic process, which involves quadrupolar degrees of freedom, is significantly dependent on small off-stoichiometry $x$ and favors all-in all-out like correlations between quadrupoles. This mechanism competes with the long range ordered quadrupolar ice, and for slightly different stoichiometry, is able to destabilize it.

cond-mat.str-el↗

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.

cond-mat.str-el↗

arXiv2020

Precise control of $J_\mathrm{eff}=1/2$ magnetic properties in Sr$_2$IrO$_4$ epitaxial thin films by variation of strain and thin film thickness

We report on a comprehensive investigation of the effects of strain and film thickness on the structural and magnetic properties of epitaxial thin films of the prototypal $J_\mathrm{eff}=1/2$ compound Sr$_2$IrO$_4$ by advanced X-ray scattering. We find that the Sr$_2$IrO$_4$ thin films can be grown fully strained up to a thickness of 108 nm. By using X-ray resonant scattering, we show that the out-of-plane magnetic correlation length is strongly dependent on the thin film thickness, but independent of the strain state of the thin films. This can be used as a finely tuned dial to adjust the out-of-plane magnetic correlation length and transform the magnetic anisotropy from two-dimensional (2D) to three-dimensional (3D) behavior by incrementing film thickness. These results provide a clearer picture for the systematic control of the magnetic degrees of freedom in epitaxial thin films of Sr$_2$IrO$_4$ and bring to light the potential for a rich playground to explore the physics of $5d$-transition metal compounds.

cond-mat.str-el↗

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.

cond-mat.str-el↗

arXiv2019

Archetypal soft-mode driven antipolar transition in francisite Cu3Bi(SeO3)2O2Cl

Model materials are precious test cases for elementary theories and provide building blocks for the understanding of more complex cases. Here, we describe the lattice dynamics of the structural phase transition in francisite Cu3Bi(SeO3)2O2Cl at 115 K and show that it provides a rare archetype of a transition driven by a soft antipolar phonon mode. In the high-symmetry phase at hightemperatures, the soft mode is found at (0,0,0.5) at the Brillouin zone boundary and is measured by inelastic X-ray scattering and thermal diffuse scattering. In the low-symmetry phase, this softmode is folded back onto the center of the Brillouin zone as a result of the doubling of the unit cell, and appears as a fully symmetric mode that can be tracked by Raman spectroscopy. On both sides of the transition, the mode energy squared follows a linear behaviour over a large temperature range. First-principles calculations reveal that, surprisingly, the flat phonon band calculated for the high-symmetry phase seems incompatible with the displacive character found experimentally. We discuss this unusual behavior in the context of an ideal Kittel model of an antiferroelectric transition.

cond-mat.mtrl-sci↗

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.

cond-mat.str-el↗

arXiv2017

Phase diagram of multiferroic KCu$_3$As$_2$O$_7$(OD)$_3$

The layered compound KCu$_3$As$_2$O$_7$(OD)$_3$, comprising distorted kagome planes of $S=1/2$ Cu$^{2+}$ ions, is a recent addition to the family of type-II multiferroics. Previous zero field neutron diffraction work has found two helically ordered regimes in \kns, each showing a distinct coupling between the magnetic and ferroelectric order parameters. Here, we extend this work to magnetic fields up to $20$~T using neutron powder diffraction, capacitance, polarization, and high-field magnetization measurements, hence determining the $H-T$ phase diagram. We find metamagnetic transitions in both low temperatures phases around $μ_0 H_c \sim 3.7$~T, which neutron powder diffraction reveals to correspond to a rotation of the helix plane away from the easy plane, as well as a small change in the propagation vector. Furthermore, we show that the sign of the ferroelectric polarization is reversible in a magnetic field, although no change is observed (or expected on the basis of the magnetic structure) due to the transition at $3.7$~T. We finally justify the temperature dependence of the polarization in both zero-field ordered phases by a symmetry analysis of the free energy expansion.

cond-mat.str-el↗

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.

cond-mat.str-el↗

arXiv2014

Magnetic order in the frustrated Ising-like chain compound Sr$_3$NiIrO$_6$

We have studied the field and temperature dependence of the magnetization of single crystals of Sr3NiIrO6. These measurements evidence the presence of an easy axis of anisotropy and two anomalies in the magnetic susceptibility. Neutron powder diffraction realized on a polycrystalline sample reveals the emergence of magnetic reflections below 75 K with magnetic propagation vector k ~ (0, 0, 1), undetected in previous neutron studies [T.N. Nguyen and H.-C zur Loye, J. Solid State Chem., 117, 300 (1995)]. The nature of the magnetic ground state, and the presence of two anomalies common to this family of material, are discussed on the basis of the results obtained by neutron diffraction, magnetization measurements, and symmetry arguments.

cond-mat.str-el↗

arXiv2014

Helical order and multiferroicity in the $S=1/2$ quasi-kagome system KCu$_3$As$_2$O$_7$(OD)$_3$

Several Cu$^{2+}$ hydroxide minerals have recently been identified as candidate realizations of the $S=1/2$ kagome Heisenberg model. In this context, we have studied the distorted system KCu$_3$As$_2$O$_7$(OD)$_3$ using neutron scattering and bulk measurements. Although the distortion favors magnetic order over a spin liquid ground state, refinement of the magnetic diffraction pattern below $T_{N1}=7.05(5)$ K yields a complex helical structure with $\mathbf{k}=(0.77~0~0.11)$. This structure, as well as the spin excitation spectrum, are well described by a classical Heisenberg model with ferromagnetic nearest neighbor couplings. Multiferroicity is observed below $T_{N1}$, with an unusual crossover between improper and pseudo-proper behavior occurring at $T_{N2}=5.5$ K. The polarization at $T=2$ K is $P=1.5 μ$Cm$^{-2}$. The properties of KCu$_3$As$_2$O$_7$(OD)$_3$ highlight the variety of physics which arise from the interplay of spin and orbital degrees of freedom in Cu$^{2+}$ kagome systems.

cond-mat.str-el↗

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.

cond-mat.str-el↗

arXiv2013

THz Magneto-electric atomic rotations in the chiral compound Ba$_3$NbFe$_3$Si$_2$O$_{14}$

We have determined the terahertz spectrum of the chiral langasite Ba$_3$NbFe$_3$Si$_2$O$_{14}$ by means of synchrotron-radiation measurements. Two excitations are revealed that are shown to have a different nature. The first one, purely magnetic, is observed at low temperature in the magnetically ordered phase and is assigned to a magnon. The second one persits far into the paramagnetic phase and exhibits both an electric and a magnetic activity at slightly different energies. This magnetoelectric excitation is interpreted in terms of atomic rotations and requires a helical electric polarization.

cond-mat.str-el↗

arXiv2013

Magnetic chirality as probed by neutron scattering

We review the concept of chirality, at first briefly in a general context then in the specific framework of the spin networks. We next discuss to what extent neutron scattering appears as an unconvertible tool to probe magnetic chirality in the static and dynamical regimes of the spins. The remarkable chiral ground state and excitations of the Fe-langasite compound finally serves to illustrate the use of neutron polarimetry in the experimental studies of the magnetic chirality.

cond-mat.str-el↗

arXiv2011

Parity Broken Chiral Spin Dynamics in Ba$_3$NbFe$_3$Si$_2$O$_{14}$

The spin wave excitations emerging from the chiral helically modulated 120$^{\circ}$ magnetic order in a langasite Ba$_3$NbFe$_3$Si$_2$O$_{14}$ enantiopure crystal were investigated by unpolarized and polarized inelastic neutron scattering. A dynamical fingerprint of the chiral ground state is obtained, singularized by (i) spectral weight asymmetries answerable to the structural chirality and (ii) a full chirality of the spin correlations observed over the whole energy spectrum. The intrinsic chiral nature of the spin waves elementary excitations is shown in absence of macroscopic time reversal symmetry breaking.

cond-mat.str-el↗

arXiv2010

Magnetoelectric MnPS3 thiophosphate as a new candidate for ferrotoroidicity

We have revisited the magnetic structure of manganese phosphorus trisulfide MnPS3 using neutron diffrac- tion and polarimetry. MnPS3 undergoes a transition toward a collinear antiferromagnetic order at 78 K. The resulting magnetic point-group breaks both the time reversal and the space inversion thus allowing a linear magnetoelectric coupling. Neutron polarimetry was subsequently used to prove that this coupling provides a way to manipulate the antiferromagnetic domains simply by cooling the sample under crossed magnetic and electrical fields, in agreement with the nondiagonal form of the magnetoelectric tensor. In addition, this tensor has, in principle, an antisymmetric part that results in a toroidic moment and provides with a pure ferrotoroidic compound.

cond-mat.str-el↗

arXiv2010

Magnetic frustration in an iron based Cairo pentagonal lattice

The Fe3+ lattice in the Bi2Fe4O9 compound is found to materialize the first analogue of a magnetic pentagonal lattice. Due to its odd number of bonds per elemental brick, this lattice, subject to first neighbor antiferromagnetic interactions, is prone to geometric frustration. The Bi2Fe4O9 magnetic properties have been investigated by macroscopic magnetic measurements and neutron diffraction. The observed non-collinear magnetic arrangement is related to the one stabilized on a perfect tiling as obtained from a mean field analysis with direct space magnetic configurations calculations. The peculiarity of this structure arises from the complex connectivity of the pentagonal lattice, a novel feature compared to the well-known case of triangle-based lattices.

cond-mat.str-el↗