arXiv subjects

S. Petit

Publications and source records attributed to S. Petit.

At least 37 records · Page 2Linked to original sources

arXiv2020

Field-angle resolved magnetic excitations as a probe of hidden-order symmetry in CeB6

In contrast to magnetic order formed by electrons' dipolar moments, ordering phenomena associated with higher-order multipoles (quadrupoles, octupoles, etc.) are more difficult to characterize because of the limited choice of experimental probes that can distinguish different multipolar moments. The heavy-fermion compound CeB6 and its La-diluted alloys are among the best-studied realizations of the long-range-ordered multipolar phases, often referred to as "hidden order". Previously the hidden order in phase II was identified as primary antiferroquadrupolar (AFQ) and field-induced octupolar (AFO) order. Here we present a combined experimental and theoretical investigation of collective excitations in the phase II of CeB6. Inelastic neutron scattering (INS) in fields up to 16.5 T reveals a new high-energy mode above 14 T in addition to the low-energy magnetic excitations. The experimental dependence of their energy on the magnitude and angle of the applied magnetic field is compared to the results of a multipolar interaction model. The magnetic excitation spectrum in rotating field is calculated within a localized approach using the pseudo-spin presentation for the Gamma8 states. We show that the rotating-field technique at fixed momentum can complement conventional INS measurements of the dispersion at constant field and holds great promise for identifying the symmetry of multipolar order parameters and the details of inter-multipolar interactions that stabilize hidden-order phases.

cond-mat.str-el↗

arXiv2019

Interplay between spin dynamics and crystal field in multiferroic compound HoMnO$_3$

In the multiferroic hexagonal manganite HoMnO3, inelastic neutron scattering and synchrotron based THz spectroscopy have been used to investigate the spin waves associated to the Mn order together with Ho crystal field excitations. While the Mn order sets in first below 80 K, a spin reorientation occurs below 37 K, a rare feature in the rare earth manganites. We show that severalHo crystal field excitations are present in the same energy range as the magnons, and that they are all affected by the spin reorientation. Moreover, several anomalous features are observed in the excitations at low temperature. Our analysis and calculations for the Mn spin waves and Ho crystal field excitations support Mn-Ho coupling mechanisms as well as coupling to the lattice affecting the dynamics.

cond-mat.mtrl-sci↗

arXiv2018

Dynamic quantum kagome ice

The search for two dimensional quantum spin liquids, exotic magnetic states with an entangled ground state remaining disordered down to zero temperature, has been a great challenge in frustrated magnetism during the last decades. Recently, fractionalized excitations, called spinons, emerging from these states, have been evidenced in kagome and triangular antiferromagnets. In contrast, quantum ferromagnetic spin liquids in two dimensions, namely quantum kagome ices, have been less investigated, yet their classical counterparts exhibit amazing properties, magnetic monopole crystals as well as magnetic fragmentation. Here we show that, by applying a magnetic field on the pyrochlore oxide Nd$_2$Zr$_2$O$_7$, which has been shown to develop three dimensional quantum magnetic fragmentation in zero field, we are able to reduce the dimension of the system and to create a dynamic kagome ice state. Our results open the way to the observation of the quantum kagome ice state which was recently investigated theoretically.

cond-mat.str-el↗

arXiv2018

Gd pyrochlore under a staggered molecular field in Gd$_2$Ir$_2$O$_7$

The influence of a staggered molecular field in frustrated rare-earth pyrochlores, produced via the magnetic iridium occupying the transition metal site, can generate exotic ground states, such as the fragmentation of the magnetization in the Ho compound. At variance with the Ising Ho$^{3+}$ moment, we focus on the behavior of the quasi isotropic magnetic moment of the Gd$^{3+}$ ion at the rare-earth site. By means of macroscopic measurements and neutron scattering, we find a complex situation where different components of the magnetic moment contribute to two antiferromagnetic non-collinear arrangements: a high temperature all in - all out order induced by the Ir molecular field, and Palmer and Chalker correlations that tend to order at much lower temperatures. This is enabled by the anisotropic nature of the Gd-Gd interactions and requires a weak easy-plane anisotropy of the Gd$^{3+}$ moment due to the mixing of the ground state with multiplets of higher spectral terms.

cond-mat.str-el↗

arXiv2018

Spin-fluctuations drive the inverse magnetocaloric effect in Mn5Si3

Inelastic neutron scattering measurements were performed on single crystals of the antiferromagnetic compound Mn5Si3 in order to investigate the relation between the spin dynamics and the magneto-thermodynamic properties. It is shown that among the two stable antiferromagnetic phases of this compound, the high temperature one has an unusual magnetic excitation spectrum where propagative spin-waves and diffuse spin-fluctuations coexist. Moreover, it is evidenced that the inverse magnetocaloric effect of Mn5Si3, the cooling by adiabatic magnetization, is associated with field induced spin-fluctuations.

cond-mat.mtrl-sci↗

arXiv2017

Long range order in the dipolar XY antiferromagnet Er$_2$Sn$_2$O$_7$

Er$_2$Sn$_2$O$_7$ remains a puzzling case among the extensively studied frustrated compounds of the rare-earth pyrochlore family. Indeed, while a first order transition towards a long-range antiferromagnetic state with the so-called Palmer-Chalker structure is theoretically predicted, it has not been observed yet, leaving the issue, as to whether it is a spin-liquid candidate, open. We report on neutron scattering and magnetization measurements which evidence a second order transition towards this Palmer-Chalker ordered state around 108 mK. Extreme care was taken to ensure a proper thermalization of the sample, which has proved to be crucial to successfully observe the magnetic Bragg peaks. At the transition, a gap opens in the excitations, superimposed on a strong quasielastic signal. The exchange parameters, refined from a spin wave analysis in applied magnetic field, confirm that Er$_2$Sn$_2$O$_7$ is a realization of the dipolar XY pyrochlore antiferromagnet. The proximity of competing phases and the strong XY anisotropy of the Er$^{3+}$ magnetic moment might be at the origin of enhanced fluctuations, leading to the unexpected nature of the transition, the low ordering temperature, and the observed multi-scale dynamics.

cond-mat.str-el↗

arXiv2017

Topological quantum phase transition in the Ising-like antiferromagnetic spin chain BaCo$_2$V$_2$O$_8$

Since the seminal ideas of Berezinskii, Kosterlitz and Thouless, topological excitations are at the heart of our understanding of a whole novel class of phase transitions. In most of the cases, those transitions are controlled by a single type of topological objects. There are however some situations, still poorly understood, where two dual topological excitations fight to control the phase diagram and the transition. Finding experimental realization of such cases is thus of considerable interest. We show here that this situation occurs in BaCo$_2$V$_2$O$_8$, a spin-1/2 Ising-like quasi-one dimensional antiferromagnet when subjected to a uniform magnetic field transverse to the Ising axis. Using neutron scattering experiments, we measure a drastic modification of the quantum excitations beyond a critical value of the magnetic field. This quantum phase transition is identified, through a comparison with theoretical calculations, to be a transition between two different types of solitonic topological objects, which are captured by different components of the dynamical structure factor.

cond-mat.str-el↗

arXiv2017

Disorder and Quantum spin ice

We report on diffuse neutron scattering experiments providing evidence for the presence of random strains in the quantum spin ice candidate Pr2Zr2O7. Since Pr is a non-Kramers ion, the strain deeply modifies the picture of Ising magnetic moments governing the low temperature properties of this material. It is shown that the derived strain distribution accounts for the temperature dependence of the specific heat and of the spin excitation spectra. Taking advantage of mean field and spin dynamics simulations, we argue that the randomness in Pr2Zr2O7, promotes a new state of matter, which is disordered, yet characterized by short range antiferroquadrupolar correlations, and from which emerge spin-ice like excitations. This study thus opens an original research route in the field of quantum spin ice.

cond-mat.str-el↗

arXiv2017

Field induced phase diagram of the XY pyrochlore antiferromagnet Er$_2$Ti$_2$O$_7$

We explore the field-temperature phase diagram of the XY pyrochlore antiferromagnet Er$_2$Ti$_2$O$_7$, by means of magnetization and neutron diffraction experiments. Depending on the field strength and direction relative to the high symmetry cubic directions $[001], [1\bar{1}0]$ and $[111]$, the refined field induced magnetic structures are derived from the zero field $ψ_2$ and $ψ_3$ states of the $Γ_5$ irreducible representation which describes the ground state of XY pyrochlore antiferromagnets. At low field, domain selection effects are systematically at play. In addition, for $[001]$, a phase transition is reported towards a $ψ_3$ structure at a characteristic field $H_c^{001}=$ 43 mT. For $[1\bar{1}0]$ and $[111]$, the spins are continuously tilted by the field from the $ψ_2$ state, and no phase transition is found while domain selection gives rise to sharp anomalies in the field dependence of the Bragg peaks intensity. For $[1\bar{1}0]$, these results are confirmed by high resolution inelastic neutron scattering experiments, which in addition allow us to determine the field dependence of the spin gap. This study agrees qualitatively with the scenario proposed theoretically by Maryasin {\it et al.} [Phys. Rev. B {\bf 93}, 100406(R) (2016)], yet the strength of the field induced anisotropies is significantly different from theory.

cond-mat.str-el↗

arXiv2017

Magnetic and dielectric order in the kagome-like francisite Cu$_3$Bi(SeO$_3$)$_2$O$_2$Cl

We report a single-crystal neutron diffraction and inelastic neutron scattering study on the spin 1/2 cuprate Cu$_3$Bi(SeO$_3$)$_2$O$_2$Cl, complemented by dielectric and electric polarization measurements. The study clarifies a number of open issues concerning this complex material, whose frustrated interactions on a kagome-like lattice, combined with Dzyaloshinskii-Moriya interactions, are expected to stabilize an exotic canted antiferromagnetic order. In particular, we determine the nature of the structural transition occurring at 115 K, the magnetic structure below 25 K resolved in the updated space group, and the microscopic ingredients at the origin of this magnetic arrangement. This was achieved by an analysis of the measured gapped spin waves, which signifies the need of an unexpected and significant anisotropic exchange beyond the proposed Dzyaloshinskii-Moriya interactions. Finally, we discuss the mutliferroic properties of this material with respect to the space group symmetries.

cond-mat.mtrl-sci↗

arXiv2017

Double Vibronic process in the quantum spin ice candidate Tb$_2$Ti$_2$O$_7$ revealed by terahertz spectroscopy

The origin of quantum fluctuations responsible for the spin liquid state in Tb$_2$Ti$_2$O$_7$ has remained a long standing problem. By synchrotron-based terahertz measurements, we show evidence of strong coupling between the magnetic and lattice degrees of freedom that provides a path to the quantum melting process. As revealed by hybrid crystal electric field-phonon excitations that appear at 0.67 THz below 200 K, and around 0.42 THz below 50 K, the double vibronic process is unique for Tb$^{3+}$ in the titanate family due to adequate energy matching and strong quadrupolar moments. The results suggest that lattice motion can indeed be the driving force behind spin flips within the hybridized ground and first excited states, promoting quantum terms in the effective Hamiltonian that describes Tb$_2$Ti$_2$O$_7$.

cond-mat.mtrl-sci↗

arXiv2017

Spin pseudogap in the $S=\frac{1}{2}$ chain material Sr$_2$CuO$_3$ with impurities

The low energy magnetic excitation spectrum of the Heisenberg antiferromagnetic $S = 1/2$ chain system Sr$_2$CuO$_3$ with Ni- and Ca-impurities is studied by neutron spectroscopy. In all cases, a defect-induced spectral pseudogap is observed and shown to scale proportionately to the number of scattering centers in the spin chains.

cond-mat.str-el↗

arXiv2016

Photoexcitation Circular Dichroism in Chiral Molecules

Chirality is ubiquitous in nature and fundamental in science, from particle physics to metamaterials.The most established technique of chiral discrimination - photoabsorption circular dichroism - relies on the magnetic properties of a chiral medium and yields an extremely weak chiral response. We propose and demonstrate a new, orders of magnitude more sensitive type of circular dichroism in neutral molecules: photoexitation circular dichroism. It does not rely on weak magnetic effects, but takes advantage of the coherent helical motion of bound electrons excited by ultrashort circularly polarized light. It results in an ultrafast chiral response and the efficient excitation of a macroscopic chiral density in an initially isotropic ensemble of randomly oriented chiral molecules. We probe this excitation without the aid of further chiral interactions using linearly polarized laser pulses. Our time-resolved study of vibronic chiral dynamics opens a way to the efficient initiation, control and monitoring of chiral chemical change in neutral molecules at the level of electrons.

physics.atm-clus↗

arXiv2016

Antiferro-quadrupolar correlations in the quantum spin ice candidate Pr2Zr2O7

We present an experimental study of the quantum spin ice candidate pyrochlore coumpound \przr\ by means of magnetization measurements, specific heat and neutron scattering up to 12 T and down to 60 mK. When the field is applied along the $[111]$ and $[1\bar{1}0]$ directions, ${\bf k}=0$ field induced structures settle in. We find that the ordered moment rises slowly, even at very low temperature, in agreement with macroscopic magnetization. Interestingly, for $H \parallel [1\bar{1}0]$, the ordered moment appears on the so called $α$ chains only. The spin excitation spectrum is essentially {\it inelastic} and consists in a broad flat mode centered at about 0.4 meV with a magnetic structure factor which resembles the spin ice pattern. For $H \parallel [1\bar{1}0]$ (at least up to 2.5 T), we find that a well defined mode forms from this broad response, whose energy increases with $H$, in the same way as the temperature of the specific heat anomaly. We finally discuss these results in the light of mean field calculations and propose a new interpretation where quadrupolar interactions play a major role, overcoming the magnetic exchange. In this picture, the spin ice pattern appears shifted up to finite energy because of those new interactions. We then propose a range of acceptable parameters for \przr\, that allow to reproduce several experimental features observed under field. With these parameters, the actual ground state of this material would be an antiferroquadrupolar liquid with spin-ice like excitations.

cond-mat.str-el↗

arXiv2016

Anisotropic interactions opposing magnetocrystalline anisotropy in Sr$_3$NiIrO$_6$

We report our investigation of the electronic and magnetic excitations of Sr$_3$NiIrO$_6$ by resonant inelastic x-ray scattering at the Ir L$_3$ edge. The intra-$t_{2g}$ electronic transitions are analyzed using an atomic model, including spin-orbit coupling and trigonal distortion of the IrO$_6$ octahedron, confronted to {\it ab initio} quantum chemistry calculations. The Ir spin-orbital entanglement is quantified and its implication on the magnetic properties, in particular in inducing highly anisotropic magnetic interactions, is highlighted. These are included in the spin-wave model proposed to account for the dispersionless magnetic excitation that we observe at 90 meV. By counterbalancing the strong Ni$^{2+}$ easy-plane anisotropy that manifests itself at high temperature, the anisotropy of the interactions finally leads to the remarkable easy-axis magnetism reported in this material at low temperature.

cond-mat.str-el↗

arXiv2016

Observation of magnetic fragmentation in spin ice

Fractionalised excitations that emerge from a many body system have revealed rich physics and concepts, from composite fermions in two-dimensional electron systems, revealed through the fractional quantum Hall effect, to spinons in antiferromagnetic chains and, more recently, fractionalisation of Dirac electrons in graphene and magnetic monopoles in spin ice. Even more surprising is the fragmentation of the degrees of freedom themselves, leading to coexisting and a priori independent ground states. This puzzling phenomenon was recently put forward in the context of spin ice, in which the magnetic moment field can fragment, resulting in a dual ground state consisting of a fluctuating spin liquid, a so-called Coulomb phase, on top of a magnetic monopole crystal. Here we show, by means of neutron scattering measurements, that such fragmentation occurs in the spin ice candidate Nd$_2$Zr$_2$O$_7$. We observe the spectacular coexistence of an antiferromagnetic order induced by the monopole crystallisation and a fluctuating state with ferromagnetic correlations. Experimentally, this fragmentation manifests itself via the superposition of magnetic Bragg peaks, characteristic of the ordered phase, and a pinch point pattern, characteristic of the Coulomb phase. These results highlight the relevance of the fragmentation concept to describe the physics of systems that are simultaneously ordered and fluctuating.

cond-mat.str-el↗

arXiv2015

Mesoscopic correlations in Tb2Ti2O7 spin liquid

We have studied the spin correlations with $\bf{k}$= ($\frac12$, $\frac12$, $\frac12$) propagation vector which appear below 0.4\, K in \tbti\ spin liquid by combining powder neutron diffraction and specific heat on Tb$_{2+x}$Ti$_{2-x}$O$_{7+y}$ samples with $x$=0, 0.01, -0.01. The $\bf{k}$= ($\frac12$, $\frac12$, $\frac12$) order clearly appears on all neutron patterns by subtracting a pattern at 1.2(1)\,K. Refining the subtracted patterns at 0.07\,K yields two possible spin structures, with spin-ice-like and monopole-like correlations respectively. Mesoscopic correlations involve Tb moments of 1 to 2 \mub\ ordered on a length scale of about 20 Å. In addition, long range order involving a small spin component of 0.1 to 0.2 \mub\ is detected for the $x$= 0 and 0.01 samples showing a peak in the specific heat. Comparison with previous single crystals data suggests that the ($\frac12$, $\frac12$, $\frac12$) order settles in through nanometric spin textures with dominant spin ice character and correlated orientations, analogous to nanomagnetic twins.

cond-mat.str-el↗

arXiv2015

Longitudinal and Transverse Zeeman Ladders in the Ising-Like Chain Antiferromagnet BaCo2V2O8

We explore the spin dynamics emerging from the Néel phase of the chain compound antiferromagnet BaCo2V2O8. Our inelastic neutron scattering study reveals unconventional discrete spin excitations, so called Zeeman ladders, understood in terms of spinon confinement, due to the interchain attractive linear potential. These excitations consist in two interlaced series of modes, respectively with transverse and longitudinal polarization. The latter have no classical counterpart and are related to the zero-point fluctuations that weaken the ordered moment in weakly coupled quantum chains. Our analysis reveals that BaCo2V2O8, with moderate Ising anisotropy and sizable interchain interactions, remarkably fulfills the conditions necessary for the observation of these longitudinal excitations.

cond-mat.str-el↗