arXiv subjects

I. Mirebeau

Publications and source records attributed to I. Mirebeau.

At least 19 recordsLinked to original sources

arXiv2021

Field-induced vortex-like textures as a probe of the critical line in reentrant spin glasses

We study the evolution of the low-temperature field-induced magnetic defects observed under an applied magnetic field in a series of frustrated amorphous ferromagnets (Fe$_{1-x}$Mn$_{x}$)$_{75}$P$_{16}$B$_{3}$Al$_{3}$ (a-FeMn). Combining small-angle neutron scattering and Monte Carlo simulations, we show that the morphology of these defects resemble that of quasi-bidimensional spin vortices. They are observed in the reentrant spin-glass (RSG) phase, up to the critical concentration $x_{\rm C} \approx 0.36$ which separates the RSG and "true" spin glass (SG) within the low temperature part of the magnetic phase diagram of a-FeMn. These vortices systematically decrease in size with increasing magnetic field or decreasing the average exchange interaction, and they finally disappear in the SG sample ($x = 0.41$), being replaced by field-induced correlations over finite length scales. We argue that the study of these nanoscopic defects could be used to probe the nature of the critical line between the RSG and SG phases.

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arXiv2019

Onset of a skyrmion phase by chemical substitution in MnGe chiral magnet

We study the evolution of the magnetic phase diagram of Mn$_{1-x}$Fe$_{x}$Ge alloys with concentration $x$ ($0 \leq x \leq 0.3$) by small-angle neutron scattering. We unambiguously observe the absence of a skyrmion lattice (or A-phase) in bulk MnGe and its onset under a small Mn/Fe substitution. The A-phase is there endowed with an exceptional skyrmion density, and is stabilized within a very large temperature region and a field range which scales with the Fe concentration. Our findings highlight the possibility to fine-tune properties of skyrmion lattices by means of chemical doping.

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arXiv2018

Spin Textures induced by Quenched Disorder in a Reentrant Spin Glass: Vortices versus "Frustrated" Skyrmions

Reentrant spin glasses are frustrated disordered ferromagnets developing vortex-like textures under an applied magnetic field. Our study of a Ni$_{0.81}$Mn$_{0.19}$ single crystal by small angle neutron scattering clarifies their internal structure and shows that these textures are randomly distributed. Spin components transverse to the magnetic field rotate over length scales of 3-15 nm in the explored field range, decreasing as field increases according to a scaling law. Monte-Carlo simulations reveal that the internal structure of the vortices is strongly distorted and differs from that assumed for "frustrated" skyrmions, built upon a competition between symmetric exchange interactions. Isolated vortices have small non-integer topological charge. The vortices keep an anisotropic shape on a 3 dimensional lattice, recalling "croutons" in a "ferromagnetic soup". Their size and number can be tuned independently by the magnetic field and concentration x (or heat treatment), respectively. This opens an original route to understand and control the influence of quenched disorder in systems hosting non trivial spin textures.

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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.

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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.

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arXiv2017

Long period helical structures and twist-grain boundary phases induced by non magnetic ion doping in Mn$_{1-x}$(Co,Rh)$_{x}$Ge chiral magnet

We study the evolution of helical magnetism in MnGe chiral magnet upon partial substitution of Mn for non magnetic 3d-Co and 4d-Rh ions. At high doping levels, we observe spin helices with very long periods -more than ten times larger than in the pure compound- and sizable ordered moments. This behavior calls for a change in the energy balance of interactions leading to the stabilization of the observed magnetic structures. Strikingly, neutron scattering unambiguously shows a double periodicity in the observed spectra at $x \gtrsim 0.45$ and $\gtrsim 0.25$ for Co- and Rh-doping, respectively. In analogy with observations made in cholesteric liquid crystals, we suggest that it reveals the presence of magnetic twist-grain-boundary phases, involving a dense short-range correlated network of screw dislocations. The dislocation cores are described as smooth textures made of non-radial double-core skyrmions.

cond-mat.mtrl-sci↗

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.

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arXiv2016

Magnetic ground state and spin fluctuations in MnGe chiral magnet as studied by Muon Spin Rotation

We have studied by muon spin resonance (μSR) the helical ground state and fluctuating chiral phase recently observed in the MnGe chiral magnet. At low temperature, the muon polarization shows double period oscillations at short time scales. Their analysis, akin to that recently developed for MnSi [A. Amato et al., Phys. Rev. B 89, 184425 (2014)], provides an estimation of the field distribution induced by the Mn helical order at the muon site. The refined muon position agrees nicely with ab initio calculations. With increasing temperature, an inhomogeneous fluctuating chiral phase sets in, characterized by two well separated frequency ranges which coexist in the sample. Rapid and slow fluctuations, respectively associated with short range and long range ordered helices, coexist in a large temperature range below T$_{N}$ = 170 K. We discuss the results with respect to MnSi, taking the short helical period, metastable quenched state and peculiar band structure of MnGe into account.

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arXiv2016

Magnetovolume effect, macroscopic hysteresis and moment collapse in the paramagnetic state of cubic MnGe under pressure

Itinerant magnets generally exhibit pressure induced transitions towards non magnetic states. Using synchrotron based X-ray diffraction and emission spectroscopy, the evolution of the lattice and spin moment in the chiral magnet MnGe was investigated in the paramagnetic state and under pressures up to 38 GPa. The collapse of spin-moment takes place in two steps. A first-order transition with a huge hysteresis around 7 GPa transforms the system from the high-spin at ambient pressure to a low-spin state. The coexistence of spin-states and observation of history-depending irreversibility is explained as effect of long-range elastic strains mediated by magnetovolume coupling. Only in a second transition, at about 23 GPa, the spin-moment collapses.

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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.

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arXiv2015

Spin dynamics in the presence of competing ferro- and antiferro-magnetic correlations in Yb2Ti2O7

In this work, we show that the zero field excitation spectra in the quantum spin ice candidate pyrochlore compound \ybti\ is a continuum characterized by a very broad and almost flat dynamical response which extends up to $1-1.5$ meV, coexisting or not with a quasi-elastic response depending on the wave-vector. The spectra do not evolve between 50 mK and 2 K, indicating that the spin dynamics is only little affected by the temperature in both the short-range correlated and ordered regimes. Although classical spin dynamics simulations qualitatively capture some of the experimental observations, we show that they fail to reproduce this broad continuum. In particular, the simulations predict an energy scale twice smaller than the experimental observations. This analysis is based on a careful determination of the exchange couplings, able to reproduce both the zero field diffuse scattering and the spin wave spectrum rising in the field polarized state. According to this analysis, \ybti\ lies at the border between a ferro and an antiferromagnetic phase. These results suggest that the unconventional ground state of \ybti\ is governed by strong quantum fluctuations arising from the competition between those phases. The observed spectra may correspond to a continuum of deconfined spinons as expected in quantum spin liquids.

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arXiv2014

Order by Disorder and Energetic Selection of the Ground State in the XY Pyrochlore Antiferromagnet Er2Ti2O7. An Inelastic Neutron Scattering Study

Examples of materials where an "order by disorder" mechanism is at play to select a particular ground state are scarce. It has recently been proposed, however, that the antiferromagnetic XY pyrochlore Er2Ti2O7, reveals a most convincing case of this mechanism. Observation of a spin gap at zone centers has recently been interpreted as a corroboration of this physics. In this paper, we argue, however, that the anisotropy generated by the interaction-induced admixing between the crystal-field ground and excited levels provides for an alternative mechanism. It especially predicts the opening of a spin gap of about 15 micro-eV, which is of the same order of magnitude as the one observed experimentally. We report new high resolution inelastic neutron scattering data which can be well understood within this scenario.

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arXiv2013

Low temperature diffuse neutron scattering and magnetisation in single crystal Tb2Ti2O7

We present an interpretation of zero field diffuse neutron scattering and of high field magnetisation data at very low temperature in the frustrated pyrochlore system Tb2Ti2O7. This material has antiferromagnetic exchange interactions and it is expected to have Ising character at low temperature. Contrary to expectations, it shows no magnetic ordering down to 0.05\,K, being thus labelled a "spin liquid". However, the ground state in Tb2Ti2O7 is not a mere fluctuating moment paramagnet but, as demonstrated by very recent experiments, a state where the electronic degrees of freedom are hybridised with the phononic variables in an unconventional way. We show here that, by approximating this complex and still unraveled electron-phonon interaction by a dynamic Jahn-Teller coupling, one can account rather well for the diffuse neutron scattering and the low temperature isothermal magnetisation. We discuss the shortcomings of this picture which arise mainly from the fact that the singlet electronic mean field ground state of the model fails to reproduce the observed strong intensity of the elastic and quasi-elastic neutron scattering.

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arXiv2013

Low temperature structural effects in the (TMTSF)$_2$PF$_6$ and AsF$_6$ Bechgaard salts

We present a detailed low-temperature investigation of the statics and dynamics of the anions and methyl groups in the organic conductors (TMTSF)$_2$PF$_6$ and (TMTSF)$_2$AsF$_6$ (TMTSF : tetramethyl-tetraselenafulvalene). The 4 K neutron scattering structure refinement of the fully deuterated (TMTSF)$_2$PF$_6$-D12 salt allows locating precisely the methyl groups at 4 K. This structure is compared to the one of the fully hydrogenated (TMTSF)$_2$PF$_6$-H12 salt previously determined at the same temperature. Surprisingly it is found that deuteration corresponds to the application of a negative pressure of 5 x 10$^2$ MPa to the H12 salt. Accurate measurements of the Bragg intensity show anomalous thermal variations at low temperature both in the deuterated PF$_6$ and AsF$_6$ salts. Two different thermal behaviors have been distinguished. Low-Bragg-angle measurements reflect the presence of low-frequency modes at characteristic energies θ$_E$ = 8.3 K and θ$_E$ = 6.7 K for the PF$_6$-D12 and AsF$_6$-D12 salts, respectively. These modes correspond to the low-temperature methyl group motion. Large-Bragg-angle measurements evidence an unexpected structural change around 55 K which probably corresponds to the linkage of the anions to the methyl groups via the formation of F...D-CD2 bonds observed in the 4 K structural refinement. Finally we show that the thermal expansion coefficient of (TMTSF)$_2$PF$_6$ is dominated by the librational motion of the PF$_6$ units. We quantitatively analyze the low-temperature variation of the lattice expansion via the contribution of Einstein oscillators, which allows us to determine for the first time the characteristic frequency of the PF6 librations: θ$_E$ = 50 K and θ$_E$ = 76 K for the PF$_6$-D12 and PF$_6$-H12 salts, respectively.

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arXiv2013

Field-induced magnetic structures in Tb2Ti2O7 spin liquid under field H || [111]

We have studied the field-induced magnetic structures of Tb2Ti2O7 pyrochlore by single-crystal neutron diffraction under a field applied along the [111] local anisotropy axis, up to H=12T and down to T=40mK. We collected a hundred magnetic Bragg peaks for each field and temperature value and refined the magnetic structures with k=0 propagation vector by performing a symmetry analysis in the space group R-3m, reducing the number of free parameters to three only. We observe a gradual reorientation of the Tb magnetic moments towards the field direction, close to a "3-in, 1-out / 1-in, 3-out" spin structure in the whole field range 0.05-12T. We perform a quantitative comparison with mean-field calculations and we propose the presence of a low-temperature dynamic symmetry breaking of the local trigonal symmetry, akin to a dynamic Jahn-Teller effect, i.e. preserving the overall cubic symmetry. We discuss the possible origin of this off-diagonal mixing term in the crystal field hamiltonian in terms of quadrupole-quadrupole interaction or magneto-elastic effects.

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arXiv2012

Effect of electron doping on the magnetic correlations in the bilayered brownmillerite compound Ca_{2.5-x}La_{x}Sr_{0.5}GaMn_{2}O_{8}: a neutron diffraction study

The effect of electron doping on the magnetic properties of the Brownmillerite-type bilayered compounds has been investigated by neutron powder diffraction in La substituted Ca2.5-xLaxSr0.5GaMn2O8 compounds (x = 0.05 and 0.1), in comparison with the undoped compound (x = 0). In all compounds, a long-range three dimensional collinear antiferromagnetic (AFM) structure is found below the Néel temperature TN of respective compound, whereas, well above TN, three dimensional short-range magnetic ordering is observed. In the intermediate temperature range just above TN, a strong effect of electron doping (La substitution) on the magnetic correlations has been observed. Here, a short-range AFM correlation with possible dimensionality of three has been found for substituted compounds (x = 0.05 and 0.1) as compared to the reported two dimensional long-range AFM ordering in the parent compound. With increasing the electron doping, a decrease in TN is also observed. The short-range magnetic correlations set in over a large temperature range above TN. A magnetic phase diagram in the x-T plane is proposed from these results.

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arXiv2012

Double-layered monopolar order in Tb2Ti2O7 spin liquid

Ho2Ti2O7 and Dy2Ti2O7 spin ices exhibit elementary excitations akin to magnetic monopoles. Here we focus on Tb2Ti2O7 spin liquid, where correlated magnetic moments keep fluctuating down to very low temperatures. Using a monopole picture, we have re-analyzed the field-induced magnetic structure previously determined by neutron diffraction in Tb2Ti2O7. We show that under a high field applied along a [110] direction, Tb2Ti2O7 orders as a three dimensional arrangement of monopole and antimonopole double layers. In contrast, Ho2Ti2O7 spin ice in the same conditions behaves as a monopole-free state. By symmetry analysis we derived the distortions compatible with the observed magnetic structure of Tb2Ti2O7 which can be related to the appearance of the double-layered monopolar order.

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arXiv2011

InMnO3 : a fully frustrated multiferroic

InMnO$_3$ is a peculiar member of the hexagonal manganites h-RMnO$_3$ (where R is a rare earth metal element), showing crystalline, electronic and magnetic properties at variance with the other compounds of the family. We have studied high quality samples synthesized at high pressure and temperature by powder neutron diffraction. The position of the Mn ions is found to be close to the threshold $\it{x}=1/3$ where superexchange Mn-Mn interactions along the $\it{c}$ axis compensate. Magnetic long range order occurs below $T_{\rm N}$= 120(2) K with a magnetic unit cell doubled along $\it{c}$, whereas short range two dimensional dynamical spin correlations are observed above $T_{\rm N}$. We propose that pseudo-dipolar interactions are responsible for the long period magnetic structure.

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