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Alexandre Bertin

Publications and source records attributed to Alexandre Bertin.

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Tilted and Twisted Magnetic Moments in the Kitaev Magnet $\alpha$-RuCl$_3$

The layered honeycomb magnet $\alpha$-RuCl$_3$ has attracted intense scrutiny as a prime candidate for realizing the Kitaev quantum spin liquid, yet a consensus on its microscopic Hamiltonian remains elusive due to the material's extreme sensitivity to structural details. Here, we report a comprehensive reexamination of the low-temperature crystallographic and magnetic structures of high-quality $\alpha$-RuCl$_3$ single crystals using unpolarized and polarized neutron diffraction. We confirm a sharp, first-order structural phase transition to the rhombohedral $R\bar{3}$ space group with a pronounced thermal hysteresis. Crucially, using both spherical and longitudinal neutron polarization analysis, we determine the 3D orientation of the ordered magnetic moment without the ambiguity typically arising from domain distributions. We find that the Ru$^{3+}$ magnetic moments in the zigzag phase are tilted by $15.7^\circ$ out of the hexagonal plane and, remarkably, exhibit an additional in-plane twist of $-13.8^\circ$. This "tilted and twisted" geometry differentiates the ground state from the previously reported models based on unpolarized neutron diffraction or resonant elastic X-ray scattering (REXS) analysis.

cond-mat.str-el

Magnetic excitations in the Kitaev material Na$_2$IrO$_3$ studied by neutron scattering

Inelastic neutron scattering experiments with a large set of comounted Na$_2$IrO$_3$ crystals reveal the low-energy magnon dispersion in this candidate material for Kitaev physics. The magnon gap amounts to 1.7(1) meV and can be interpreted similarly to the sister compound $\alpha$-RuCl$_{3}$ to stem from the zone boundaries in the antiferromagnetic zigzag structure. The neutron experiments find no evidence for low-energy excitations with ferromagnetic character, which contrasts to the findings in $\alpha$-RuCl$_{3}$. Our results are consistent with a recently proposed microscopic model that involves an antiferromagnetic Heisenberg nearest-neighbor exchange in Na$_2$IrO$_3$ in contrast to the ferromagnetic one considered for $\alpha$-RuCl$_{3}$. Although the magnetic response shows the signatures of bond-directional anisotropy in both materials the different relative signs of Kitaev and Heisenberg interaction result in different deviations from the initial Kitaev model. Low-energy ferromagnetic fluctuations cannot be considered as a fingerprint of ferromagnetic Kitaev interaction.

cond-mat.str-el

Crystal structure and absence of magnetic order in single crystalline RuO$_2$

RuO$_2$ was considered for a long time to be a paramagnetic metal with an ideal rutile-type structure down to low temperatures, but recent studies on single-crystals claimed evidence for antiferromagnetic order and some symmetry breaking in the crystal structure. We have grown single-crystals of RuO2 by vapor transport using either O$_2$ or TeCl$_4$ as transport medium. These crystals exhibit metallic behavior following a $T^2$ low-temperature relation and a small paramagnetic susceptibility that can be attributed to Pauli paramagnetism. Neither the conductance nor the susceptibility measurements yield any evidence for a magnetic or a structural transition between 300K and $\sim$4 K. Comprehensive single-crystal diffraction studies with neutron and X-ray radiation reveal the rutile structure to persist until 2K in our crystals, and show nearly perfect stoichiometry. Previous observations of symmetry forbidden reflections can be attributed to multiple diffraction. Polarized single-crystal neutron diffraction experiments at 1.6K exclude the proposed antiferromagnetic structures with ordered moments larger than 0.01 Bohr magnetons.

cond-mat.mtrl-sci

Direct evidence for anisotropic magnetic interaction in $\alpha$-RuCl$_3$ from polarized inelastic neutron scattering

Polarized neutron scattering experiments reveal the anisotropy of magnetic correlations in the candidate Kitaev material $\alpha$-RuCl$_3$. The anisotropy of the inelastic response at the magnetic Bragg positions is just opposite to the expectation for a simple Heisenberg model. Near the antiferromagnetic $q$ vector, there are no low-energy transversal magnon modes directly documenting the fully anisotropic and bond-directional character of the magnetic interaction in $\alpha$-RuCl$_3$. However, other findings disagree with a simple or strongly dominant Kitaev component.

cond-mat.str-el

Interplay of magnetic order and ferroelasticity in the spin-orbit coupled antiferromagnet K$_2$ReCl$_6$

The magnetic and structural phase transitions occurring in K$_2$ReCl$_6$ were studied by macroscopic and microscopic techniques. Structural phase transitions associated with rotations of the ReCl$_6$ octahedra lower the symmetry from cubic to monoclinic, form ferroelastic domains, and are visible in susceptibility, specific heat and thermal expansion measurements. In the antiferromagnetically ordered state slightly below $T_{\rm N}$=12\,K these domains can be rearranged by a magnetic field inducing a relative elongation of the polydomain crystal parallel to the field of 0.6\%. At zero field the magnetic structure in K$_2$ReCl$_6$ does not exhibit a weak ferromagnetic component, but at large magnetic field a distinct magnetic structure with a finite weak ferromagnetic component is stabilized. High magnetic fields rearrange the domains in the crystal to align the weak ferromagnetic moment parallel to the field. The altered domain structure with the crystal elongation is abruptly suppressed at lower temperature but persists upon heating to well above $T_{\rm N}$. However, heating above the lowest structural phase transition and successive cooling restore the initial shape.

cond-mat.str-el

Rearrangement of uncorrelated valence bonds evidenced by low-energy spin excitations in YbMgGaO4

DC-magnetization data measured down to 40 mK speak against conventional freezing and reinstate YbMgGaO$_4$ as a triangular spin-liquid candidate. Magnetic susceptibility measured parallel and perpendicular to the $c$-axis reaches constant values below 0.1 and 0.2 K, respectively, thus indicating the presence of gapless low-energy spin excitations. We elucidate their nature in the triple-axis inelastic neutron scattering experiment that pinpoints the low-energy ($E$ $\leq$ $J_0$ $\sim$ 0.2 meV) part of the excitation continuum present at low temperatures ($T$ $<$ $J_0$/$k_B$), but \emph{completely} disappearing upon warming the system above $T$ $\gg$ $J_0$/$k_B$. In contrast to the high-energy part at $E$ $>$ $J_0$ that is rooted in the breaking of nearest-neighbor valence bonds and persists to temperatures well above $J_0$/$k_B$, the low-energy one originates from the rearrangement of the valence bonds and thus from the propagation of unpaired spins. We further extend this picture to herbertsmithite, the spin-liquid candidate on the kagome lattice, and argue that such a hierarchy of magnetic excitations may be a universal feature of quantum spin liquids.

cond-mat.str-el