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J. Gaudet

Publications and source records attributed to J. Gaudet.

At least 19 recordsLinked to original sources

Incommensurate magnetic order drives singular angular magnetoresistance in a Weyl semimetal

We demonstrate that a multi-$\mathbf{k}$ incommensurate magnetic state in the Weyl semimetal CeAlGe gives rise to singular angular magnetoresistance (SAMR), an electrical-transport signature that detects the magnetic-field direction with exceptional precision. In contrast, the sister compound CeAlSi shows neither multi-$\mathbf{k}$ order nor SAMR. Both phenomena emerge upon $\sim57\%$ Ge substitution in CeAlSi$_{1-x}$Ge$_x$ and coincide with electronic-structure changes that soften the single-ion in-plane anisotropy and enhance Weyl-mediated magnetic interactions. These results reveal a direct connection between band topology, electronic transport, and collective magnetism in Weyl semimetals.

cond-mat.str-el

Intertwined Charge and Spin Density Waves in a Topological Kagome Material

Using neutrons and x-rays we show the topological kagome antiferromagnet Mn$_3$Sn for $T<285$~K forms a homogeneous spin and charge ordered state comprising a longitudinally polarized spin density wave (SDW) with wavevector $\textbf{k}_β=k_β{\bf \hat{c}}$, a helical modulated version of the room temperature anti-chiral magnetic order with $\textbf{k}_χ=k_χ{\bf \hat{c}}$, and charge density waves with wave vectors $2\textbf{k}_β, 2\textbf{k}_χ$, and $\textbf{k}_β+\textbf{k}_χ$. Though $\textbf{k}_χ$ and $\textbf{k}_β$ coincide for $200~{\rm K}<T<230$~K, they exhibit distinct continuous $T-$dependencies before locking to commensurate values of $\textbf{k}_β = \frac{1}{12}\textbf{c}^{*}$ and $\textbf{k}_χ = \frac{5}{48}\textbf{c}^{*}$ at low$-T$. Density functional theory indicates this complex modulated state may be associated with the nesting of Fermi surfaces from correlated flat kagome bands, which host Weyl nodes that are annihilated as it forms.

cond-mat.str-el

Quantum Spin Ice Response to a Magnetic Field in the Dipole-Octupole Pyrochlore Ce$_2$Zr$_2$O$_7$

We report new heat capacity measurements on single crystal Ce$_2$Zr$_2$O$_7$ down to $\sim$ 0.1 K in a magnetic field along the $[1,\bar{1}, 0]$ direction. These new measurements show that the broad hump in the zero-field heat capacity moves higher in temperature with increasing field strength and is split into two humps by the $[1,\bar{1}, 0]$ field at $\sim$ 2 T. These separate features are due to the decomposition of the pyrochlore lattice into effectively decoupled chains for fields in this direction: one set of chains ($α$-chains) is polarized by the field while the other ($β$-chains) remains free. Our theoretical modelling suggests that the $β$-chains are close to a critical state, with nearly-gapless excitations. We also report new elastic and inelastic neutron scattering measurements on single crystal Ce$_2$Zr$_2$O$_7$ in $[1, \bar{1}, 0]$ and $[0, 0, 1]$ magnetic fields at temperatures down to 0.03 K. The elastic scattering behaves consistently with the formation of independent chains for a $[1, \bar{1}, 0]$ field, while the $[0, 0, 1]$ field produces a single field-induced magnetic Bragg peak at $(0, 2, 0)$ and equivalent wavevectors, indicating a polarized spin ice for fields above $\sim$ 3 T. For both $[1, \bar{1}, 0]$ and $[0, 0, 1]$ fields, our inelastic neutron scattering results show an approximately-dispersionless continuum of scattering that increases in both energy and intensity with increasing field strength. By modelling the complete set of experimental data using numerical linked cluster and semiclassical molecular dynamics calculations, we demonstrate the dominantly multipolar nature of the exchange interactions in Ce$_2$Zr$_2$O$_7$ and the smallness of the parameter $θ$ which controls the mixing between dipolar and octupolar degrees of freedom. These results support previous estimates of the microscopic exchange parameters.

cond-mat.str-el

Spin-orbital order and excitons in magnetoresistive HoBi

The magnetism of the rock-salt $fcc$ rare-earth monopnictide HoBi, a candidate topological material with extreme magnetoresistance, is investigated. From the Ho$^{3+}$ non-Kramers $J$=8 spin-orbital multiplet, the cubic crystal electric field yields six nearly degenerate low-energy levels. These constitute an anisotropic magnetic moment with a Jahn-Teller-like coupling to the lattice. In the cubic phase for $T>T_N~=~5.72(1)~K$, the paramagnetic neutron scattering is centered at $\mathbf{k}=(\frac{1}{2}\frac{1}{2}\frac{1}{2})$ and was fit to dominant antiferromagnetic interactions between Ho spins separated by $\{100\}$ and ferromagnetic interactions between spins displaced by $\{\frac{1}{2}\frac{1}{2}0\}$. For $T<T_N$, a type-II AFM long-range order with $\mathbf{k}=(\frac{1}{2}\frac{1}{2}\frac{1}{2})$ develops along with a tetragonal lattice distortion. While neutron diffraction from a multi-domain sample cannot unambiguously determine the spin orientation within a domain, the bulk magnetization, structural distortion, and our measurements of the magnetic excitations all show the easy axis coincides with the tetragonal axis. The weakly dispersive excitons for $T<T_N$ can be accounted for by a spin Hamiltonian that includes the crystal electric field and exchange interactions within the Random Phase Approximation.

cond-mat.str-el

Reply to "Comment on: 'Case for a U(1)$_π$ Quantum Spin Liquid Ground State in the Dipole-Octupole Pyrochlore $\mathrm{Ce}_2\mathrm{Zr}_2\mathrm{O}_7$' "

In his comment [arXiv:2209.03235], S. W. Lovesey argues that our analysis of neutron scattering experiments performed on Ce$_2$Zr$_2$O$_7$ is invalid. Lovesey argues that we have not properly accounted for the higher-order multipolar contributions to the magnetic scattering and that our use of pseudospin-$1/2$ operators to describe the scattering is inappropriate. In this reply, we show that the multipolar corrections discussed by Lovesey only become significant at scattering wavevectors exceeding those accessed in our experiments. This in no way contradicts or undermines our work, which never claimed a direct observation of scattering from higher-order multipoles. We further show that Lovesey's objections to our use of pseudospins are unfounded, and that the pseudospin operators are able to describe all magnetic scattering processes at the energy scale of our experiments, far below the crystal field gap. Finally, we comment on certain assumptions in Lovesey's calculations of the scattering amplitude which are inconsistent with experiment.

cond-mat.str-el

Incommensurate magnetic orders and topological Hall effect in the square-net centrosymmetric EuGa$_2$Al$_2$ system

Neutron diffraction on the centrosymmetric square-net magnet EuGa$_2$Al$_2$ reveals multiple incommensurate magnetic states (AFM1,2,3) in zero field. In applied field, a new magnetic phase (A) is identified from magnetization and transport measurements, bounded by two of the $μ_0H$~=~0 incommensurate magnetic phases (AFM1,helical and AFM3, cycloidal) with different moment orientations. Moreover, magneto-transport measurements indicate the presence of a topological Hall effect, with maximum values centered in the A phase. Together, these results render EuGa$_2$Al$_2$ a material with non-coplanar or topological spin texture in applied field. X-ray diffraction reveals an out-of-plane (OOP) charge density wave (CDW) below $T_{CDW} \sim$ 50 K while the magnetic propagation vector lies in plane below $T_N$ = 19.5 K. Together these data point to a new route to realizing in-plane non-collinear spin textures through an OOP CDW. In turn, these non-collinear spin textures may be unstable against the formation of topological spin textures in an applied field.

cond-mat.str-el

The case for a U(1)$_\pi$ Quantum Spin Liquid Ground State in the Dipole-Octupole Pyrochlore Ce$_2$Zr$_2$O$_7$

The Ce$^{3+}$ pseudospin-$\frac{1}{2}$ degrees of freedom in the pyrochlore magnet Ce$_2$Zr$_2$O$_7$ are known to possess dipole-octupole (DO) character, making it a candidate for novel quantum spin liquid (QSL) ground states at low temperatures. We report new polarized neutron diffraction at low temperatures, as well as heat capacity ($C_p$) measurements on single crystal Ce$_2$Zr$_2$O$_7$. The former bears both similarities and differences from that measured in the canonical dipolar spin ice compound Ho$_2$Ti$_2$O$_7$, while the latter rises sharply at low temperatures, initially plateauing near 0.08 K, before falling off towards a high temperature zero beyond 3 K. Above $\sim$0.5 K, the $C_p$ data set can be fit to the results of a quantum numerical linked cluster (NLC) calculation, carried out to 4$^{\mathrm{th}}$ order, that allows estimates for the terms in the near-neighbour XYZ Hamiltonian expected for such DO pyrochlore systems. Fits of the same theory to the temperature dependence of the magnetic susceptibility and unpolarized neutron scattering complement this analysis. A comparison between the resulting best fit NLC calculation and the polarized neutron diffraction shows both agreement and discrepancies, mostly in the form of zone-boundary diffuse scattering in the non-spin flip channel, which are attributed to interactions beyond near-neighbours. The lack of an observed thermodynamic anomaly and the constraints on the near-neighbour XYZ Hamiltonian suggest that Ce$_2$Zr$_2$O$_7$ realizes a U(1)$_\pi$ QSL state at low temperatures, and one that likely resides near the boundary between dipolar and octupolar character.

cond-mat.str-el

Intertwined Magnetic Dipolar and Electric Quadrupolar Correlations in the Pyrochlore Tb$_2$Ge$_2$O$_7$

We present a comprehensive experimental and theoretical study of the pyrochlore Tb$_2$Ge$_2$O$_7$, an exemplary realization of a material whose properties are dominated by competition between magnetic dipolar and electric quadrupolar correlations. The dipolar and quadrupolar correlations evolve over three distinct regimes that we characterize via heat capacity, elastic and inelastic neutron scattering. In the first regime, above $T^*=1.1$ K, significant quadrupolar correlations lead to an intense inelastic mode that cannot be accounted for within a scenario with solely magnetic dipole-dipole correlations. The onset of extended dipole correlations occurs in the intermediate regime, between $T^*=1.1$ K and $T_c = 0.25$ K, with the formation of a collective paramagnetic state characterized by extended ferromagnetic canted spin ice domains. Here, long-range order is impeded not only by the usual frustration operating in classical spin ice systems, but also by a competition between dipolar and quadrupolar correlations. Finally, in the lowest temperature regime, below $T_c=0.25$ K, there is an abrupt and significant increase in the dipole ordered moment. The majority of the ordered moment remains tied up in the ferromagnetic spin ice-like state, but an additional $\mathbf{k}=(0,0,1)$ antiferromagnetic order parameter also develops. Simultaneously, the spectral weight of the inelastic mode, which is a proxy for the quadrupolar correlations, is observed to drop, indicating that dipole order ultimately wins out. Tb$_2$Ge$_2$O$_7$ is therefore a remarkable platform to study intertwined dipolar and quadrupolar correlations in a magnetically frustrated system and provides important insights into the physics of the whole family of terbium pyrochlores.

cond-mat.str-el

Low Energy Magneto-optics of Tb$_{2}$Ti$_{2}$O$_{7}$ in [111] Magnetic Field

The pyrochlore magnet Tb$_{2}$Ti$_{2}$O$_{7}$ shows a lack of magnetic order to low temperatures and is considered to be a quantum spin liquid candidate. We perform time-domain THz spectroscopy on high quality Tb$_{2}$Ti$_{2}$O$_{7}$ crystal and study the low energy excitations as a function of [111] magnetic field with high energy resolution. The low energy crystal field excitations change their energies anomalously under magnetic field. Despite several sharp field dependent changes, we show that the material's spectrum can be described not by a phase transitions, but by field dependent hybridization between the low energy crystal field levels. We highlight the strong coupling between spin and lattice degrees of freedom in Tb$_{2}$Ti$_{2}$O$_{7}$ as evidenced by the magnetic field tunable crystal field environment. Calculations based on single ion physics with field induced symmetry reduction of the crystal field environment can reproduce our data.

cond-mat.str-el

Antichiral spin order its Goldstone modes and their hybridization with phonons in the topological semimetal Mn3Ge

Quantum materials with strong transport responses to disparate physical quantities are of great fundamental significance and may hold technological potentials. The interplay between interactions and topology drive such responses through the effects of spontaneous symmetry breaking and the associated domain configurations on quantum transport. Here we provide a comprehensive description of the magnetism of Mn3Ge, an antiferromagnetic kagomebased semimetal with room temperature transport anomalies associated with topologically protected Weyl nodes. Using polarized neutron diffraction, we show the all-important magnetic structure is anti-chiral and coplanar carrying the symmetry of a ferromagnet without appreciable magnetization. We probe and classify the long wavelength excitations that determine its macroscopic responses including a set of collective magneto-elastic modes. We develop a phenomenological spin Hamiltonian with exchange, Dzyaloshinskii-Moriya, and crystal field interactions to describe its collective magnetism. The itinerant character of the magnetism that drives quantum transport is apparent in spin wave damping and extended magnetic interactions. Our work provides the scientific basis for manipulation of the chiral antiferromagnetic texture of Mn3Ge to control its topological quantum transport.

cond-mat.str-el

Quantum Spin Ice Dynamics in the Dipole-Octupole Pyrochlore Magnet Ce$_2$Zr$_2$O$_7$

Neutron scattering measurements on the pyrochlore magnet Ce$_2$Zr$_2$O$_7$ reveal an unusual crystal field splitting of its lowest $J$=5/2 multiplet, such that its ground state doublet is composed of m$_J$=$\pm$3/2, giving these doublets a dipole - octupole (DO) character with local Ising anisotropy. Its magnetic susceptibility shows weak antiferromagnetic correlations with $θ_{CW}$=-0.4(2)K, leading to a naive expectation of an All-In, All-Out ordered state at low temperatures. Instead our low energy inelastic neutron scattering measurements show a dynamic quantum spin ice state, with suppressed scattering near |$\textbf{Q}$|=0, and no long range order at low temperatures. This is consistent with recent theory predicting symmetry enriched U(1) quantum spin liquids for such DO doublets decorating the pyrochlore lattice. Finally, we show that disorder, especially oxidation of powder samples, is important in Ce$_2$Zr$_2$O$_7$ and could play an important role in the low temperature behaviour of this material.

cond-mat.str-el

Interplay of Magnetism and Transport in HoBi

We report the observation of an extreme magnetoresistance (XMR) in HoBi with a large magnetic moment from Ho f-electrons. Neutron scattering is used to determine the magnetic wave vectors across several metamagnetic (MM) transitions on the phase diagram of HoBi. Unlike other magnetic rare-earth monopnictides, the field dependence of resistivity in HoBi is non-monotonic and reveals clear signatures of every metamagnetic transition in the low-temperature and low-field regime, at T < 2 K and H < 2.3 T. The XMR appears at H > 2.3 T after all the metamagnetic transitions are complete and the system is spin-polarized by the external magnetic field. The existence of an onset field for XMR and the intimate connection between magnetism and transport in HoBi are unprecedented among the magnetic rare-earth monopnictides. Therefore, HoBi provides a unique opportunity to understand the electrical transport in magnetic XMR semimetals.

cond-mat.mtrl-sci

Dipolar-Octupolar Ising Antiferromagnetism in Sm$_2$Ti$_2$O$_7$: A Moment Fragmentation Candidate

Over the past two decades, the magnetic ground states of all rare earth titanate pyrochlores have been extensively studied, with the exception of Sm$_2$Ti$_2$O$_7$. This is, in large part, due to the very high absorption cross-section of naturally-occurring samarium, which renders neutron scattering infeasible. To combat this, we have grown a large, isotopically-enriched single crystal of Sm$_2$Ti$_2$O$_7$. Using inelastic neutron scattering, we determine that the crystal field ground state for Sm$^{3+}$ is a dipolar-octupolar doublet with Ising anisotropy. Neutron diffraction experiments reveal that Sm$_2$Ti$_2$O$_7$ orders into the all-in, all-out magnetic structure with an ordered moment of 0.44(7) $μ_B$ below $T_N=0.35$ K, consistent with expectations for antiferromagnetically-coupled Ising spins on the pyrochlore lattice. Zero-field muon spin relaxation measurements reveal an absence of spontaneous oscillations and persistent spin fluctuations down to 0.03 K. The combination of the dipolar-octupolar nature of the Sm$^{3+}$ moment, the all-in, all-out ordered state, and the low-temperature persistent spin dynamics make this material an intriguing candidate for moment fragmentation physics.

cond-mat.str-el

Magneto-elastic induced vibronic bound state in the spin ice pyrochlore Ho$_2$Ti$_2$O$_7$

The single ion physics of Ho$_2$Ti$_2$O$_7$ is well-understood to produce strong Ising anisotropy, which is an essential ingredient to its low-temperature spin ice state. We present inelastic neutron scattering measurements on Ho$_2$Ti$_2$O$_7$ that reveal a clear inconsistency with its established single ion Hamiltonian. Specifically, we show that a crystal field doublet near 60~meV is split by approximately 3~meV. Furthermore, this crystal field splitting is not isolated to Ho$_2$Ti$_2$O$_7$ but can also be found in its chemical pressure analogs, Ho$_2$Ge$_2$O$_7$ and Ho$_2$Sn$_2$O$_7$. We demonstrate that the origin of this effect is a vibronic bound state, resulting from the entanglement of a phonon and crystal field excitation. We derive the microscopic Hamiltonian that describes the magneto-elastic coupling and provides a quantitative description of the inelastic neutron spectra.

cond-mat.str-el

Anomalous metamagnetism in the low carrier density Kondo lattice YbRh3Si7

We report complex metamagnetic transitions in single crystals of the new low carrier Kondo antiferromagnet YbRh3Si7. Electrical transport, magnetization, and specific heat measurements reveal antiferromagnetic order at T_N = 7.5 K. Neutron diffraction measurements show that the magnetic ground state of YbRh3Si7 is a collinear antiferromagnet where the moments are aligned in the ab plane. With such an ordered state, no metamagnetic transitions are expected when a magnetic field is applied along the c axis. It is therefore surprising that high field magnetization, torque, and resistivity measurements with H||c reveal two metamagnetic transitions at mu_0H_1 = 6.7 T and mu_0H_2 = 21 T. When the field is tilted away from the c axis, towards the ab plane, both metamagnetic transitions are shifted to higher fields. The first metamagnetic transition leads to an abrupt increase in the electrical resistivity, while the second transition is accompanied by a dramatic reduction in the electrical resistivity. Thus, the magnetic and electronic degrees of freedom in YbRh3Si7 are strongly coupled. We discuss the origin of the anomalous metamagnetism and conclude that it is related to competition between crystal electric field anisotropy and anisotropic exchange interactions.

cond-mat.str-el

Long-wavelength correlations in ferromagnetic titanate pyrochlores as revealed by small angle neutron scattering

We have carried out small angle neutron scattering measurements on single crystals of two members of the family of cubic rare-earth titanate pyrochlores that display ferromagnetic Curie-Weiss susceptibilities,Yb$_2$Ti$_2$O$_7$ and Ho$_2$Ti$_2$O$_7$. Ho$_2$Ti$_2$O$_7$ is established as displaying a prototypical classical dipolar spin ice ground state, while Yb$_2$Ti$_2$O$_7$ has been purported as a candidate for a quantum spin ice ground state. While both materials have been well studied with neutron scattering techniques, neither has been previously explored in single crystal form with small angle neutron scattering (SANS). Our results for Yb$_2$Ti$_2$O$_7$ show distinct SANS features below its $Θ_{CW}$$\sim$ 0.50 K, with rods of diffuse scattering extending along $\langle 111 \rangle$ directions in reciprocal space, off-rod scattering which peaks in temperature near $Θ_{CW}$, and quasi-Bragg scattering at very small angles which correlates well with T$_C$ $\sim$ 0.26 K. The quasi-Bragg scattering corresponds to finite extent ferromagnetic domains $\sim$ 140 Å$~$ across, at the lowest temperatures. We interpret the $\langle 111\rangle$ rods of diffuse scattering as arising from domain boundaries between the finite-extent ferromagnetic domains. In contrast the SANS signal in Ho$_2$Ti$_2$O$_7$ is isotropic within the (HHL) plane around $\textbf{Q}$=0. However the strength of this overall SANS signal has a temperature dependence resembling that of the magnetic heat capacity, with a peak near 3 K. Below the break between the field-cooled and the zero-field cooled susceptibility in Ho$_2$Ti$_2$O$_7$ at $\sim$ 0.60 K, the SANS signal is very low, approaching zero.

cond-mat.str-el

Phase Competition in the Palmer-Chalker XY Pyrochlore Er$_2$Pt$_2$O$_7$

We report neutron scattering measurements on Er$_2$Pt$_2$O$_7$, a new addition to the XY family of frustrated pyrochlore magnets. Symmetry analysis of our elastic scattering data shows that Er$_2$Pt$_2$O$_7$ is the first XY pyrochlore to order into the $k=0$, $Γ_7$ magnetic structure (the Palmer-Chalker state), at $T_N = 0.38$ K. This contrasts with its sister XY pyrochlore antiferromagnets Er$_2$Ti$_2$O$_7$ and Er$_2$Ge$_2$O$_7$, both of which order into $Γ_5$ magnetic structures at much higher temperatures, $T_N=1.2$ K and $1.4$ K, respectively. In this temperature range, the magnetic heat capacity of Er$_2$Pt$_2$O$_7$ contains a broad anomaly centered at $T^*=1.5$ K. Our inelastic neutron scattering measurements reveal that this broad heat capacity anomaly sets the temperature scale for strong short-range spin fluctuations. Below $T_N = 0.38$ K, Er$_2$Pt$_2$O$_7$ displays a gapped spin wave spectrum with an intense, flat band of excitations at lower energy and a weak, diffusive band of excitations at higher energy. The flat band is well-described by classical spin wave calculations, but these calculations also predict sharp dispersive branches at higher energy, a striking discrepancy with the experimental data. This, in concert with the strong suppression of $T_N$, is attributable to enhanced quantum fluctuations due to phase competition between the $Γ_7$ and $Γ_5$ states that border each other within a classically predicted phase diagram.

cond-mat.str-el

Effect of Chemical Pressure on the Crystal Electric Field States of Erbium Pyrochlore Magnets

We have carried out a systematic study of the crystal electric field excitations in the family of cubic pyrochlores Er$_2B_2$O$_7$, with $B=$~Ti, Ge, Pt, and Sn, using neutron spectroscopy. All members of this family are magnetic insulators based on 4$f^{11}$ Er$^{3+}$ and non-magnetic $B^{4+}$. At sufficiently low temperatures, long-range antiferromagnetic order is observed in each of these Er$_2B_2$O$_7$ pyrochlores. Our inelastic neutron scattering measurements probe the transitions from the ground state doublet to excited crystal electric field states belonging to the $J=15/2$ Hund's rules manifold. This allows us to quantitatively determine the energy eigenvalues and eigenfunctions of these $(2J+1)=16$ states across the Er$_2B_2$O$_7$ series. The different ionic sizes associated with different non-magnetic $B^{4+}$ cations correspond to positive or negative chemical pressure, depending on the relative contraction or expansion of the crystal lattice, which gives rise to slightly different local environments at the Er$^{3+}$ site. Our results show that the $g$-tensor components, which characterize the anisotropy of the ground state doublet eigenfunctions, are XY-like for all four members of the Er$_2B_2$O$_7$ series. However, the XY anisotropy is much stronger for Er$_2$Pt$_2$O$_7$ and Er$_2$Sn$_2$O$_7$ ($\frac{g_{\perp}}{g_z} > 25$), than for Er$_2$Ge$_2$O$_7$ and Er$_2$Ti$_2$O$_7$ ($\frac{g_{\perp}}{g_z} < 4$). The variation in the nature of the XY-anisotropy in these systems correlates strongly with their ground states, as Er$_2$Ge$_2$O$_7$ and Er$_2$Ti$_2$O$_7$ order into $Γ_5$ magnetic structures, while Er$_2$Pt$_2$O$_7$ and Er$_2$Sn$_2$O$_7$ order in the $Γ_7$ Palmer-Chalker structure.

cond-mat.str-el