arXiv subjects

E. Lhotel

Publications and source records attributed to E. Lhotel.

At least 37 records · Page 2Linked to original sources

arXiv2021

Experimental measurement of the isolated magnetic susceptibility

The isolated susceptibility $χ_{\rm I}$ may be defined as a (non-thermodynamic) average over the canonical ensemble, but while it has often been discussed in the literature, it has not been clearly measured. Here, we demonstrate an unambiguous measurement of $χ_{\rm I}$ at avoided nuclear-electronic level crossings in a dilute spin ice system, containing well-separated holmium ions. We show that $χ_{\rm I}$ quantifies the superposition of quasi-classical spin states at these points, and is a direct measure of state concurrence and populations.

quant-ph↗

arXiv2020

Metastable and localized Ising magnetism in $α$-CoV$_{2}$O$_{6}$ magnetization plateaus

$α$-CoV$_{2}$O$_{6}$ consists of $j_{\mathrm{eff}}={1 \over 2}$ Ising spins located on an anisotropic triangular motif with magnetization plateaus in an applied field. We combine neutron diffraction with low temperature magnetization to investigate the magnetic periodicity in the vicinity of these plateaus. We find these steps to be characterized by metastable and spatially short-range ($ξ\sim$ 10 $Å$) magnetic correlations with antiphase boundaries defining a local periodicity of $\langle \hat{T}^{2} \rangle =\ \uparrow \downarrow$ to $\langle \hat{T}^{3} \rangle =\ \uparrow \uparrow \downarrow$, and $\langle \hat{T}^{4} \rangle=\ \uparrow \uparrow \downarrow \downarrow$ or $\uparrow \uparrow \uparrow \downarrow$ spin arrangements. This shows the presence of spatially short range and metastable/hysteretic, commensurate magnetism in Ising magnetization steps.

cond-mat.str-el↗

arXiv2020

Fragmented monopole crystal, dimer entropy and Coulomb interactions in Dy$_2$Ir$_2$O$_7$

Neutron scattering, specific heat and magnetisation measurements on both powders and single crystals reveal that Dy$_2$Ir$_2$O$_7$ realizes the fragmented monopole crystal state in which antiferromagnetic order and a Coulomb phase spin liquid co-inhabit. The measured residual entropy is that of a hard core dimer liquid, as predicted. Inclusion of Coulomb interactions allows for a quantitative description of both the thermodynamic data and the magnetisation dynamics, with the energy scale given by deconfined defects in the emergent ionic crystal. Our data reveal low energy excitations, as well as a large distribution of energy barriers down to low temperatures, while the magnetic response to an applied field suggests that domain wall pinning is important; results that call for further theoretical modelling.

cond-mat.str-el↗

arXiv2019

Nuclear spin assisted quantum tunnelling of magnetic monopoles in spin ice

Extensive work on single molecule magnets has identified a fundamental mode of relaxation arising from the nuclear-spin assisted quantum tunnelling of nearly independent and quasi-classical magnetic dipoles. Here we show that nuclear-spin assisted quantum tunnelling can also control the dynamics of purely emergent excitations: magnetic monopoles in spin ice. Our low temperature experiments were conducted on canonical spin ice materials with a broad range of nuclear spin values. By measuring the magnetic relaxation, or monopole current, we demonstrate strong evidence that dynamical coupling with the hyperfine fields bring the electronic spins associated with magnetic monopoles to resonance, allowing the monopoles to hop and transport magnetic charge. Our result shows how the coupling of electronic spins with nuclear spins may be used to control the monopole current. It broadens the relevance of the assisted quantum tunnelling mechanism from single molecular spins to emergent excitations in a strongly correlated system.

cond-mat.str-el↗

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

Pauling entropy, metastability and equilibrium in Dy$_2$Ti$_2$O$_7$ spin ice

Determining the fate of the Pauling entropy in the classical spin ice material Dy$_2$Ti$_2$O$_7$ with respect to the third law of thermodynamics has become an important test case for understanding the existence and stability of ice-rule states in general. The standard model of spin ice - the dipolar spin ice model - predicts an ordering transition at $T\approx 0.15$ K, but recent experiments by Pomaranski $et\ al.$ suggest an entropy recovery over long time scales at temperatures as high as $0.5$ K, much too high to be compatible with theory. Using neutron scattering and specific heat measurements at low temperatures and with long time scales ($0.35$ K$/10^6$ s and $0.5$ K$/10^5$ s respectively) on several isotopically enriched samples we find no evidence of a reduction of ice-rule correlations or spin entropy. High-resolution simulations of the neutron structure factor show that the spin correlations remain well described by the dipolar spin ice model at all temperatures. Further, by careful consideration of hyperfine contributions, we conclude that the original entropy measurements of Ramirez $et\ al.$ are, after all, essentially correct: the short-time relaxation method used in that study gives a reasonably accurate estimate of the equilibrium spin ice entropy due to a cancellation of contributions.

cond-mat.str-el↗

arXiv2018

Absence of magnetic ordering and field induced phase diagram in the Gadolinium Aluminium garnet

The robustness of spin liquids with respect to small perturbations, and the way magnetic frustration can be lifted by slight changes in the balance between competing magnetic interactions remains a rich and open issue. We address this question through the study of the Gadolinium Aluminium garnet Gd$_3$Al$_5$O$_{12}$, a related compound to the extensively studied Gd$_3$Ga$_5$O$_{12}$. We report on its magnetic properties at very low temperature. We show that despite a freezing at about 300 mK, no magnetic transition is observed, suggesting the presence of a spin liquid state down to the lowest temperatures similarly to Gd$_3$Ga$_5$O$_{12}$, in spite of a larger ratio between exchange and dipolar interactions. Finally, the phase diagram as a function of field and temperature is strongly reminiscent from the one reported in Gd$_3$Ga$_5$O$_{12}$. This study reveals the robust nature of the spin liquid phase for Gd ions on the garnet lattice in stark contrast to Gd ions on the pyrochlore lattice for which a slight perturbation drives the compound into a range of magnetically ordered states.

cond-mat.str-el↗

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

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

Experimental signature of the attractive Coulomb force between positive and negative magnetic monopoles in spin ice

A non-Ohmic current that grows exponentially with the square root of applied electric field is well known from thermionic field emission (the Schottky effect), electrolytes (the second Wien effect) and semiconductors (the Poole-Frenkel effect). It is a universal signature of the attractive Coulomb force between positive and negative electrical charges, which is revealed as the charges are driven in opposite directions by the force of an applied electric field. Here we apply thermal quenches to spin ice to prepare metastable populations of bound pairs of positive and negative emergent magnetic monopoles at millikelvin temperatures. We find that the application of a magnetic field results in a universal exponential-root field growth of magnetic current, thus confirming the microscopic Coulomb force between the magnetic monopole quasiparticles and establishing a magnetic analogue of the Poole-Frenkel effect. At temperatures above 300 mK, gradual restoration of kinetic monopole equilibria causes the non-Ohmic current to smoothly evolve into the high field Wien effect for magnetic monopoles, as confirmed by comparison to a recent and rigorous theory of the Wien effect in spin ice. Our results extend the universality of the exponential-root field form into magnetism and illustrate the power of emergent particle kinetics to describe far-from equilibrium response in complex systems.

cond-mat.str-el↗

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

Magnetic charge injection in spin ice: a new way to fragmentation

The complexity embedded in condensed matter fertilizes the discovery of new states of matter, enriched by ingredients like frustration. Illustrating examples in magnetic systems are Kitaev spin liquids, skyrmions phases, or spin ices. These unconventional ground states support exotic excitations, for example the magnetic charges in spin ices, also called monopoles. Beyond their discovery, an important challenge is to be able to control and manipulate them. Here, we propose a new mechanism to inject monopoles in a spin ice through a staggered magnetic field. We show theoretically, and demonstrate experimentally in the Ho$_2$Ir$_2$O$_7$ pyrochlore iridate, that it results in the stabilization of a monopole crystal, which exhibits magnetic fragmentation. In this new state of matter, the magnetic moment fragments into an ordered part and a persistently fluctuating one. Compared to conventional spin ices, the different nature of the excitations in this fragmented state opens the way to novel tunable field-induced and dynamical behaviors.

cond-mat.str-el↗

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

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

Evidence for unidimensional low-energy excitations as the origin of persistent spin dynamics in geometrically frustrated magnets

We report specific heat, magnetic, and muon spin relaxation measurements performed on a polycrystalline sample of the normal spinel CdHo2S4. The rare-earth ions sit on a lattice of corner-sharing regular tetrahedra as in pyrochlore compounds. Magnetic ordering is detected at Tc ~ 0.87 K. From spin-lattice relaxation rate measurements on both sides of Tc we uncover similar magnetic excitation modes driving the so-called persistent spin dynamics at T < Tc. Unidimensional excitations are argued to be at its origin. Often observed spin loop structures are suggested to support these excitations. The possibility of a generic mechanism for their existence is discussed.

cond-mat.str-el↗

arXiv2015

Fluctuations and all-in$-$all-out ordering in dipole-octupole Nd2Zr2O7

We present an experimental study of the pyrochlore coumpound Nd2Zr2O7 by means of neutron scattering and magnetization measurements down to 90 mK. The Nd$^{3+}$ magnetic moments exhibit a strong local $\langle$111$\rangle$ Ising anisotropy together with a dipolar-octupolar nature, different from the standard Kramers-doublet studied so far. We show that, despite the positive Curie-Weiss temperature, \ndzr\ undergoes a transition around 285 mK towards an all-in$-$all-out antiferromagnetic state. We establish the $(H,T)$ phase diagram in the three directions of the applied field and reveal a metamagnetic transition around 0.1 T. The strongly reduced ordered magnetic moment as well as the unexpected shape of the magnetization curves demonstrate that Nd2Zr2O7 , is not a standard Ising antiferromagnet. We propose that the peculiar nature of the Nd doublet combined with competing interactions explain these findings.

cond-mat.str-el↗