The composition dependence of the structural transition between the monoclinic $1{T}^{\ensuremath{'}}$ and orthorhombic ${T}_{d}$ phases in the ${\mathrm{Mo}}_{1\ensuremath{-}x}{\mathrm{W}}_{x}{\mathrm{Te}}_{2}$ Weyl semimetal was investigated by elastic neutron scattering on single crystals up to $x\ensuremath{\approx}0.54$. First observed in ${\mathrm{MoTe}}_{2}$, the transition from ${T}_{d}$ to $1{T}^{\ensuremath{'}}$ is accompanied by an intermediate pseudo-orthorhombic phase, ${T}_{d}^{*}$. Upon doping with W, the ${T}_{d}^{*}$ phase vanishes by $x\ensuremath{\approx}0.34$. Above this concentration, a phase coexistence behavior with both ${T}_{d}$ and $1{T}^{\ensuremath{'}}$ is observed instead. The interlayer in-plane positioning parameter $\ensuremath{\delta}$, which relates to the $1{T}^{\ensuremath{'}}\phantom{\rule{4pt}{0ex}}\ensuremath{\beta}$ angle, decreases with temperature as well as with W substitution, likely due to strong anharmonicity in the interlayer interactions. The temperature width of the phase coexistence remains almost constant up to $x\ensuremath{\approx}0.54$, in contrast to the broadening reported under pressure.
Spontaneous symmetry breaking—the phenomenon in which an infinitesimal perturbation can cause the system to break the underlying symmetry—is a cornerstone concept in the understanding of interacting solid-state systems. In a typical series of temperature-driven phase transitions, higher-temperature phases are more symmetric due to the stabilizing effect of entropy that becomes dominant as the temperature is increased. However, the opposite is rare but possible when there are multiple degrees of freedom in the system. Here, we present such an example of a symmetry-ascending phenomenon upon cooling in a magnetic kagome metal FeGe by utilizing neutron Larmor diffraction and Raman spectroscopy. FeGe has a kagome lattice structure with simple A-type antiferromagnetic order below Néel temperature TN≈400K and a charge density wave (CDW) transition at TCDW≈110K, followed by a spin-canting transition at around 60 K. In the paramagnetic state at 460 K, we confirm that the crystal structure is indeed a hexagonal kagome lattice. On cooling to around TN, the crystal structure changes from hexagonal to monoclinic with in-plane lattice distortions on the order of 10−4 and the associated splitting of the double-degenerate phonon mode of the pristine kagome lattice. Upon further cooling to TCDW, the kagome lattice shows a small negative thermal expansion, and the crystal structure gradually becomes more symmetric upon further cooling. A tendency of increasing the crystalline symmetry upon cooling is unusual; it originates from an extremely weak structural instability that coexists and competes with the CDW and magnetic orders. These observations are against the expectations for a simple model with a single order parameter and hence can only be explained by a Landau free energy expansion that takes into account multiple lattice, charge, and spin degrees of freedom. Thus, the determination of the crystalline lattice symmetry as well as the unusual spin-lattice coupling is a first step towards understanding the rich electronic and magnetic properties of the system, and it sheds new light on intertwined orders where the lattice degree of freedom is no longer dominant. Published by the American Physical Society 2024
Spin-triplet superconductors are of extensive current interest because they can host topological state and Majorana fermions important for quantum computation. The uranium-based heavy-fermion superconductor ${\mathrm{UTe}}_{2}$ has been argued as a spin-triplet superconductor similar to ${\mathrm{UGe}}_{2}$, URhGe, and UCoGe, where the superconducting phase is near (or coexists with) a ferromagnetic (FM) instability and spin-triplet electron pairing is driven by FM spin fluctuations. Here we use neutron scattering to show that, although ${\mathrm{UTe}}_{2}$ exhibits no static magnetic order down to 0.3 K, its magnetism in the [$0,K,L$] plane is dominated by incommensurate spin fluctuations near an antiferromagnetic ordering wave vector and extends to at least 2.6 meV. We are able to understand the dominant incommensurate spin fluctuations of ${\mathrm{UTe}}_{2}$ in terms of its electronic structure calculated using a combined density-functional and dynamic mean-field theory.
Abstract Triangular lattice of rare-earth ions with interacting effective spin-1/2 local moments is an ideal platform to explore the physics of quantum spin liquids (QSLs) in the presence of strong spin-orbit coupling, crystal electric fields, and geometrical frustration. The Yb delafossites, NaYb Ch 2 ( Ch =O, S, Se) with Yb ions forming a perfect triangular lattice, have been suggested to be candidates for QSLs. Previous thermodynamics, nuclear magnetic resonance, and powder sample neutron scattering measurements on NaYb Ch 2 have supported the suggestion of the QSL ground states. The key signature of a QSL, the spin excitation continuum, arising from the spin quantum number fractionalization, has not been observed. Here we perform both elastic and inelastic neutron scattering measurements as well as detailed thermodynamic measurements on high-quality single crystalline NaYbSe 2 samples to confirm the absence of long-range magnetic order down to 40 mK, and further reveal a clear signature of magnetic excitation continuum extending from 0.1 to 2.5 meV. By comparing the structure of our magnetic excitation spectra with the theoretical expectation from the spinon continuum, we conclude that the ground state of NaYbSe 2 is a QSL with a spinon Fermi surface.
Using elastic neutron scattering on single crystals of MoTe$_{2}$ and Mo$_{1-x}$W$_{x}$Te$_{2}$ ($x \lesssim 0.01$), the temperature dependence of the recently discovered T$_{d}^{*}$ phase, present between the low temperature orthorhombic T$_{d}$ phase and high temperature monoclinic 1T$^{\prime}$ phase, is explored. The T$_{d}^{*}$ phase appears only on warming from T$_{d}$ and is observed in the hysteresis region prior to the 1T$^{\prime}$ transition. This phase consists of four layers in its unit cell, and is constructed by an "AABB" sequence of layer stacking operations rather than the "AB" and "AA" sequences of the 1T$^{\prime}$ and T$_{d}$ phases, respectively. Though the T$_{d}^{*}$ phase emerges without disorder on warming from T$_{d}$, on cooling from 1T$^{\prime}$ diffuse scattering is observed that suggests a frustrated tendency toward the "AABB" stacking.
Magnetic order in most materials occurs when magnetic ions with finite moments arrange in a particular pattern below the ordering temperature. Intriguingly, if the crystal electric field (CEF) effect results in a spin-singlet ground state, a magnetic order can still occur due to the exchange interactions between neighboring ions admixing the excited CEF levels. The magnetic excitations in such a state are spin excitons generally dispersionless in reciprocal space. Here we use neutron scattering to study stoichiometric Ni2Mo3O8, where Ni2+ ions form a bipartite honeycomb lattice comprised of two triangular lattices, with ions subject to the tetrahedral and octahedral crystalline environment, respectively. We find that in both types of ions, the CEF excitations have nonmagnetic singlet ground states, yet the material has magnetic order. Furthermore, CEF spin excitons from the tetrahedral sites form a dispersive diffusive pattern around the Brillouin zone boundary, likely due to spin entanglement and geometric frustrations.
Triangular lattice of rare-earth ions with interacting effective spin-1/2 local moments is an ideal platform to explore the physics of quantum spin liquids (QSLs) in the presence of strong spin-orbit coupling, crystal electric fields, and geometrical frustration. The Yb delafossites, NaYbCh2 (Ch=O, S, Se) with Yb ions forming a perfect triangular lattice, have been suggested to be candidates for QSLs. Previous thermodynamics, nuclear magnetic resonance, and powder-sample neutron scattering measurements on NaYbCh2 have supported the suggestion of the QSL ground states. The key signature of a QSL, the spin excitation continuum, arising from the spin quantum number fractionalization, has not been observed. Here we perform both elastic and inelastic neutron scattering measurements as well as detailed thermodynamic measurements on high-quality single-crystal NaYbSe2 samples to confirm the absence of long-range magnetic order down to 40 mK, and further reveal a clear signature of magnetic excitation continuum extending from 0.1 to 2.5 meV. The comparison between the structure of the magnetic excitation spectra and the theoretical expectation from the spinon continuum suggests that the ground state of NaYbSe2 is a QSL with a spinon Fermi surface.Received 23 December 2020Revised 30 March 2021Accepted 8 April 2021DOI:https://doi.org/10.1103/PhysRevX.11.021044Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.Published by the American Physical SocietyPhysics Subject Headings (PhySH)Research AreasAntiferromagnetismQuantum spin liquidSpinonCondensed Matter, Materials & Applied Physics
Spontaneous symmetry breaking-the phenomenon where an infinitesimal perturbation can cause the system to break the underlying symmetry-is a cornerstone concept in the understanding of interacting solid-state systems. In a typical series of temperature-driven phase transitions, higher temperature phases are more symmetric due to the stabilizing effect of entropy that becomes dominant as the temperature is increased. However, the opposite is rare but possible when there are multiple degrees of freedom in the system. Here, we present such an example of a symmetry-ascending phenomenon in a magnetic kagome metal FeGe by utilizing neutron Larmor diffraction and Raman spectroscopy. In the paramagnetic state at 460K, we confirm that the crystal structure is indeed hexagonal kagome lattice. On cooling to TN, the crystal structure changes from hexagonal to monoclinic with in-plane lattice distortions on the order of 10^(-4) and the associated splitting of the double degenerate phonon mode of the pristine kagome lattice. Upon further cooling to TCDW, the kagome lattice shows a small negative thermal expansion, and the crystal structure becomes more symmetric gradually upon further cooling. Increasing the crystalline symmetry upon cooling is unusual, it originates from an extremely weak structural instability that coexists and competes with the CDW and magnetic orders. These observations are against the expectations for a simple model with a single order parameter, hence can only be explained by a Landau free energy expansion that takes into account multiple lattice, charge, and spin degrees of freedom. Thus, the determination of the crystalline lattice symmetry as well as the unusual spin-lattice coupling is a first step towards understanding the rich electronic and magnetic properties of the system and sheds new light on intertwined orders where the lattice degree of freedom is no longer dominant.
Quantum spin liquid (QSL) is a disordered state of quantum-mechanically entangled spins commonly arising from frustrated magnetic dipolar interactions. However, QSL in some pyrochlore magnets can also come from frustrated magnetic octupolar interactions. Although the key signature for both dipolar and octupolar interaction-driven QSL is the presence of a spin excitation continuum (spinons) arising from the spin quantum number fractionalization, an external magnetic field-induced ferromagnetic order will transform the spinons into conventional spin waves in a dipolar QSL. By contrast, in an octupole QSL, the spin waves carry octupole moments that do not couple, in the leading order, to an external magnetic field or to neutron moments but will contribute to the field dependence of the heat capacity. Here we use neutron scattering to show that the application of a large external magnetic field to ${\mathrm{Ce}}_{2}{\mathrm{Zr}}_{2}{\mathrm{O}}_{7}$, an octupolar QSL candidate, induces an Anderson-Higgs transition by condensing the spinons into a static ferromagnetic ordered state with octupolar spin waves invisible to neutrons but contributing to the heat capacity. Our theoretical calculations also provide a microscopic, qualitative understanding for the presence of octupole scattering at large wave vectors in ${\mathrm{Ce}}_{2}{\mathrm{Sn}}_{2}{\mathrm{O}}_{7}$ pyrochlore, and its absence in ${\mathrm{Ce}}_{2}{\mathrm{Zr}}_{2}{\mathrm{O}}_{7}$. Therefore, our results identify ${\mathrm{Ce}}_{2}{\mathrm{Zr}}_{2}{\mathrm{O}}_{7}$ as a strong candidate for an octupolar $U(1)$ QSL, establishing that frustrated magnetic octupolar interactions are responsible for QSL properties in Ce-based pyrochlore magnets.
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