arXiv subjects

Martin Mourigal

Publications and source records attributed to Martin Mourigal.

36 records · Page 2Linked to original sources

arXiv2022

LiYbSe2: Frustrated Magnetism in a New Pyrochlore Lattice

Three-dimensionally (3D) frustrated magnets generally exist in the magnetic diamond and pyrochlore lattices, in which quantum fluctuations suppress magnetic orders and generate highly entangled ground states (GS). LiYbSe2 in a previously unreported pyrochlore lattice was discovered from LiCl flux growth. Distinct from the quantum spin liquid (QSL) candidate NaYbSe2 hosting a perfect triangular lattice of Yb3+, LiYbSe2 crystallizes in the cubic pyrochlore structure with space group Fd-3m (No. 227). The Yb3+ ions in LiYbSe2 are arranged on a network of corner-sharing tetrahedra, which is particularly susceptible to geometrical frustration. According to our temperature-dependent magnetic susceptibility measurements, the dominant antiferromagnetic interaction in LiYbSe2 is expected to appear around 8 K. However, no long-range magnetic order is detected in thermomagnetic measurements above 70 mK. Specific heat measurements also show magnetic correlations shifting with applied magnetic field with a degree of missing entropy that may be related to the slight mixture of Yb3+ on the Li site. Such magnetic frustration of Yb3+ is rare in pyrochlore structures. Thus, LiYbSe2 shows promises in intrinsically realizing disordered quantum states like QSL in pyrochlore structures.

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arXiv2022

Anticollinear order and degeneracy lifting in square lattice antiferromagnet LaSrCrO4

We report the static and dynamic magnetic properties of LaSrCrO$_4$, a seemingly canonical spin-3/2 square-lattice antiferromagnet that exhibits frustration between magnetic layers -- owing to their AB stacking -- and offers a rare testbed to investigate accidental-degeneracy lifting in magnetism. Neutron diffraction experiments on single-crystal samples uncover a remarkable anticollinear magnetic order below $T_N$ = 170 K characterized by a Néel arrangement of the spins within each layer and an orthogonal arrangement between adjacent layers. To understand the origin of this unusual magnetic structure, we analyze the spin-wave excitation spectrum by means of inelastic neutron scattering and bulk measurements. A spectral gap of 0.5 meV, along with a spin-flop transition at 3.2\, T, reflect the energy scale associated with the degeneracy-lifting. A minimal model to explain these observations requires both a positive biquadratic interlayer exchange and dipolar interactions, both of which are on the order of 10$^{-4}$ meV, only a few parts per million of the dominant exchange interaction $J_1 \approx 11$ meV. These results provide direct evidence for the selection of a non-collinear magnetic structure by the combined effect of two distinct degeneracy lifting interactions.

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arXiv2021

Magneto-transport evidence for strong topological insulator phase in ZrTe5

The identification of a non-trivial band topology usually relies on directly probing the protected surface/edge states. But, it is difficult to achieve electronically in narrow-gap topological materials due to the small (meV) energy scales. Here, we demonstrate that band inversion, a crucial ingredient of the non-trivial band topology, can serve as an alternative, experimentally accessible indicator. We show that an inverted band can lead to a four-fold splitting of the non-zero Landau levels, contrasting the two-fold splitting (spin splitting only) in the normal band. We confirm our predictions in magneto-transport experiments on a narrow-gap strong topological insulator, zirconium pentatelluride (ZrTe$_5$), with the observation of additional splittings in the quantum oscillations and also an anomalous peak in the extreme quantum limit. Our work establishes an effective strategy for identifying the band inversion as well as the associated topological phases for future topological materials research.

cond-mat.mtrl-sci↗

arXiv2021

Magnetic properties and signatures of moment ordering in triangular lattice antiferromagnet KCeO$_2$

The magnetic ground state and the crystalline electric field level scheme of the triangular lattice antiferromagnet KCeO$_2$ are investigated. Below $T_N =$ 300 mK, KCeO$_2$ develops signatures of magnetic order in specific heat measurements and low energy inelastic neutron scattering data. Trivalent Ce$^{3+}$ ions in the $D_{3d}$ local environment of this compound exhibit large splittings among the lowest three $4f^1$ Kramers doublets defining for the free ion the $J = 5/2$ sextet and a ground state doublet with dipole character, consistent with recent theoretical predictions in M. S. Eldeeb et al. Phys. Rev. Materials 4, 124001 (2020). An unexplained, additional local mode appears, and potential origins of this anomalous mode are discussed.

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arXiv2021

Effective point-charge analysis of crystal electric fields -- application to rare-earth pyrochlores and tripod kagome magnets R3Mg2Sb3O14

An indispensable step to understand collective magnetic phenomena in rare-earth compounds is the determination of spatially-anisotropic single-ion properties resulting from spin-orbit coupling and crystal field (CF). The CF Hamiltonian has a discrete energy spectrum -- accessible to spectroscopic probes such as neutron scattering -- controlled by a number of independent parameters reflecting the point-symmetry of the magnetic sites. Determining these parameters in low-symmetry systems is often challenging. Here, we describe a general method to analyze CF excitation spectra using adjustable effective point-charges. We benchmark our method to existing neutron-scattering measurements on pyrochlore rare-earth oxides and obtain a universal point-charge model that describes a large family of related materials. We adapt this model to the newly discovered tripod Kagome magnets ($R_{3}$Mg$_2$Sb$_{3}$O$_{14}$, $R$ = Tb, Ho, Er, Yb) for which we report broadband inelastic neutron-scattering spectra. Analysis of these data using adjustable point-charges yields the CF wave-functions for each compound. From this, we calculate thermomagnetic properties that accurately reflect our measurements on powder samples, and predict the effective gyromagnetic tensor for pseudo-spin degrees of freedom -- a crucial step to understand the exotic collective properties of these kagome magnets at low temperature. We present further applications of our method to other tripod kagome materials and triangular rare-earth compounds $R$MgGaO$_4$ ($R$ =Yb, Tm). Overall, this study establishes a widely applicable methodology to predict CF and single-ion properties of rare-earth compounds based on interpretable and adjustable models of effective point-charges.

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arXiv2021

Neutron scattering investigation of proposed Kosterlitz-Thouless transitions in the triangular-lattice Ising antiferromagnet TmMgGaO4

The transverse-field Ising model on the triangular lattice is expected to host an intermediate finite-temperature Kosterlitz-Thouless (KT) phase through a mapping of the spins on each triangular unit to a complex order parameter. TmMgGaO$_4$ is a candidate material to realize such physics due to the non-Kramers nature of Tm$^{3+}$ ion and the resulting two-singlet single-ion ground state. Using inelastic neutron scattering, we confirm this picture by determining the leading parameters of the low-energy effective Hamiltonian of TmMgGaO$_4$. Subsequently, we track the predicted KT phase and related transitions by inspecting the field and temperature dependence of the ac susceptibility. We further probe the spin correlations in both reciprocal space and real space via single crystal neutron diffraction and magnetic total scattering techniques, respectively. Magnetic pair distribution function analysis provides evidence for the formation of vortex-antivortex pairs that characterize the proposed KT phase around 5~K. Although structural disorder influences the field-induced behavior of TmMgGaO$_4$, the magnetism in zero field appears relatively free from these effects. These results position TmMgGaO$_4$ as a strong candidate for a solid-state realization of KT physics in a dense spin system.

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arXiv2020

Observation of 4- and 6-magnon bound-states in the spin-anisotropic frustrated antiferromagnet FeI$_2$

Spin-waves e.g. magnons are the conventional elementary excitations of ordered magnets. However, other possibilities exist. For instance, magnon bound-states can arise due to attractive magnon-magnon interactions and drastically impact the static and dynamic properties of materials. Here, we demonstrate a zoo of distinct multi-magnon quasiparticles in the frustrated spin-1 triangular antiferromagnet FeI$_2$ using time-domain terahertz spectroscopy. The energy-magnetic field excitation spectrum contains signatures of one-, two-, four- and six-magnon bound-states, which we analyze using an exact diagonalization approach for a dilute gas of interacting magnons. The two-magnon single-ion bound states occur due to strong anisotropy and the preponderance of even higher order excitations arises from the tendency of the single-ion bound states to themselves form bound states due to their very flat dispersion. This menagerie of tunable interacting quasiparticles provides a unique platform in a condensed matter setting that is reminiscent of the few-body quantum phenomena central to cold-atom, nuclear, and particle physics experiments.

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arXiv2020

Collective excitations in the tetravalent lanthanide honeycomb antiferromagnet, Na2PrO3

Thermomagnetic and inelastic neutron scattering measurements on Na2PrO3 are reported. This material is an antiferromagnetic honeycomb magnet based on the tetravalent lanthanide Pr4+ and has been proposed to host dominant antiferromagnetic Kitaev interactions. These measurements reveal magnetic fluctuations in Na2PrO3 below an energy of 2 meV as well as crystal-field excitations around 230 meV. The latter energy is comparable to the scale of the spin-orbit interaction and explains both the very small effective moment of around 1.0 μB per Pr4+ and the difficulty to uncover any static magnetic scattering below the ordering transition at TN = 4.6 K. By comparing the low-energy magnetic excitations in Na2PrO3 to that of the isostructural spin-only compound, Na2TbO3, a microscopic model of exchange interactions is developed that implicates dominant and surprisingly large Heisenberg exchange interactions J approximately equal to 1.1(1) meV. Although antiferromagnetic Kitaev interactions with K less than or equal to 0.2J cannot be excluded, the inelastic neutron scattering data of Na2PrO3 is best explained with a delta = 1.24(2) easy-axis XXZ exchange anisotropy.

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arXiv2020

Quantum versus Classical Spin Fragmentation in Dipolar Kagome Ice Ho3Mg2Sb3O14

A promising route to realize entangled magnetic states combines geometrical frustration with quantum-tunneling effects. Spin-ice materials are canonical examples of frustration, and Ising spins in a transverse magnetic field are the simplest many-body model of quantum tunneling. Here, we show that the tripod kagome lattice material Ho${_3}$Mg${_2}$Sb${_3}$O${_{14}}$ unites an ice-like magnetic degeneracy with quantum-tunneling terms generated by an intrinsic splitting of the Ho$^{3+}$ ground-state doublet, which is further coupled to a nuclear spin bath. Using neutron scattering and thermodynamic experiments, we observe a symmetry-breaking transition at $T^{\ast}\approx0.32$ K to a remarkable state with three peculiarities: a concurrent recovery of magnetic entropy associated with the strongly coupled electronic and nuclear degrees of freedom; a fragmentation of the spin into periodic and ice-like components; and persistent inelastic magnetic excitations down to $T\approx0.12$ K. These observations deviate from expectations of classical spin fragmentation on a kagome lattice, but can be understood within a model of dipolar kagome ice under a homogeneous transverse magnetic field, which we survey with exact diagonalization on small clusters and mean-field calculations. In Ho${_3}$Mg${_2}$Sb${_3}$O${_{14}}$, hyperfine interactions dramatically alter the single-ion and collective properties, and suppress possible quantum correlations, rendering the fragmentation with predominantly single-ion quantum fluctuations. Our results highlight the crucial role played by hyperfine interactions in frustrated quantum magnets, and motivate further investigations of the role of quantum fluctuations on partially-ordered magnetic states.

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arXiv2020

A Novel Magnetic Material by Design: Observation of Yb3+ with Spin-1/2 and Possible Superconducting Trace in YbxPt5P

The localized f-electrons enrich the magnetic properties in rare-earth-based intermetallics. Among those, compounds with heavier 4d and 5d transition metals are even more fascinating because anomalous electronic properties may be induced by the hybridization of 4f and itinerant conduction electrons primarily from the d orbitals. Here, we describe the observation of trivalent Yb3+ with S = 1/2 at low temperatures in YbxPt5P, the first of a new family of materials. YbxPt5P (0.20< x <1) phases were synthesized and structurally characterized. They exhibit a large homogeneity width with the Yb ratio exclusively occupying the 1a site in the anti-CeCoIn5 structure. Moreover, the resistivity measurement of a sample analyzed as Yb0.25Pt5P shows it to exist a complete zero-resistance transition with a critical transition temperature of ~0.6 K, possible superconductivity. However, the zero-resistivity transition was not observed in YbPt5P with antiferromagnetic ordering existing solely. First-principles electronic structure calculations substantiate the antiferromagnetic ground state and indicate that 2D nesting around the Fermi level may give rise to exotic physical properties, such as superconductivity. YbxPt5P appears to be a unique case among materials.

cond-mat.mtrl-sci↗

arXiv2020

Stripe antiferromagnetic ground state of ideal triangular lattice KErSe$_2$

Rare earth triangular lattice materials have been proposed as a good platform for the investigation of frustrated magnetic ground states. KErSe$_2$ with the delafossite structure, contains perfect two-dimensional Er$^{3+}$ triangular layers separated by potassium ions, realizing this ideal configuration and inviting study. Here we investigate the magnetism of KErSe$_2$ at miliKelvin temperatures by heat capacity and neutron powder diffraction. Heat capacity results reveal a magnetic transition at 0.2 K in zero applied field. This long-range order is suppressed by an applied magnetic field of 0.5 T below 0.08 K. Neutron powder diffraction suggests that the zero-field magnetic structure orders with $k=(\frac{1}{2},0,\frac{1}{2})$ in a stripe spin structure. Unexpectedly, Er is found to have a reduced moment of 3.06(1) $μ_B$/Er in the ordered state and diffuse magnetic scattering, which originates at higher temperatures, is found to persist in the ordered state potentially indicating magnetic fluctuations. Neutron diffraction collected under an applied field shows a metamagnetic transition at $\sim$ 0.5 T to ferromagnetic order with $k$=(0,0,0) and two possible structures, which are likely dependent on the applied field direction. First principle calculations show that the zero field stripe spin structure can be explained by the first, second and third neighbor couplings in the antiferromagnetic triangular lattice.

cond-mat.mtrl-sci↗

arXiv2020

Hybridized quadrupolar excitations in the spin-anisotropic frustrated magnet FeI2

Magnetic order is usually associated with well-defined magnon excitations. Exotic magnetic fluctuations with fractional, topological or multipolar character, have been proposed for radically different forms of magnetic matter such as spin-liquids. As a result, considerable efforts have searched for, and uncovered, low-spin materials with suppressed dipolar order at low temperatures. Here, we report neutron-scattering experiments and quantitative theoretical modeling of an exceptional spin-1 system -- the uniaxial triangular magnet FeI2 -- where a bright and dispersive band of mixed dipolar-quadrupolar fluctuations emerges just above a dipolar ordered ground-state. This excitation arises from anisotropic exchange interactions that hybridize overlapping modes carrying fundamentally different quantum numbers. Remarkably, a generalization of spin-wave theory to local SU(3) degrees of freedom accounts for all details of the low-energy dynamical response of FeI2 without going beyond quadratic order. Our work highlights that quantum excitations without classical counterparts can be realized even in presence of fully developed magnetic order.

cond-mat.str-el↗

arXiv2019

Modeling Spin Dynamics in the Singlet Ground State Garnet Ho3Ga5O12

Materials containing non-Kramers magnetic ions can show unusual quantum excitations because of the exact mapping of the two-singlet crystal-field ground state to a quantum model of Ising spins in a transverse magnetic field. Here, we model the magnetic excitation spectrum of garnet-structured Ho3Ga5O12, which has a two-singlet crystal-field ground state. We use a reaction-field approximation to explain published inelastic neutron-scattering data [Zhou et al., Phys. Rev. B 78, 140406(R) (2008)] using a three-parameter model containing the magnetic dipolar interaction, the two-singlet crystal-field splitting, and the nuclear hyperfine coupling. Our study clarifies the magnetic Hamiltonian of Ho3Ga5O12, reveals that the nuclear hyperfine interaction drives magnetic ordering in this system, and provides a framework for quantitative analysis of magnetic excitation spectra of materials with singlet crystal-field ground states.

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arXiv2019

Evidence for a quantum dipole liquid state in an organic quasi-two-dimensional material

Mott insulators are commonly pictured with electrons localized on lattice sites. Their low-energy degrees of freedom involve spins only. Here we observe emerging charge degrees of freedom in a molecule-based Mott insulator $κ$-(BEDT-TTF)$_2$Hg(SCN)$_2$Br, resulting in a quantum dipole liquid state. Electrons localized on molecular dimer lattice sites form electric dipoles that do not order at low temperatures and fluctuate with frequency detected experimentally in our Raman spectroscopy experiments. The heat capacity and Raman scattering response are consistent with a scenario where the composite spin and electric dipole degrees of freedom remain fluctuating down to the lowest measured temperatures.

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arXiv2018

Quantum Spin Fragmentation in Kagome Ice Ho3Mg2Sb3O14

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arXiv2018

Hierarchy of exchange interactions in the triangular-lattice spin-liquid YbMgGaO$_{4}$

The spin-1/2 triangular lattice antiferromagnet YbMgGaO$_{4}$ has attracted recent attention as a quantum spin-liquid candidate with the possible presence of off-diagonal anisotropic exchange interactions induced by spin-orbit coupling. Whether a quantum spin-liquid is stabilized or not depends on the interplay of various exchange interactions with chemical disorder that is inherent to the layered structure of the compound. We combine time-domain terahertz spectroscopy and inelastic neutron scattering measurements in the field polarized state of YbMgGaO$_{4}$ to obtain better microscopic insights on its exchange interactions. Terahertz spectroscopy in this fashion functions as high-field electron spin resonance and probes the spin-wave excitations at the Brillouin zone center, ideally complementing neutron scattering. A global spin-wave fit to all our spectroscopic data at fields over 4T, informed by the analysis of the terahertz spectroscopy linewidths, yields stringent constraints on $g$-factors and exchange interactions. Our results paint YbMgGaO$_{4}$ as an easy-plane XXZ antiferromagnet with the combined and necessary presence of sub-leading next-nearest neighbor and weak anisotropic off-diagonal nearest-neighbor interactions. Moreover, the obtained $g$-factors are substantially different from previous reports. This works establishes the hierarchy of exchange interactions in YbMgGaO$_{4}$ from high-field data alone and thus strongly constrains possible mechanisms responsible for the observed spin-liquid phenomenology.

cond-mat.str-el↗

arXiv2016

Emergent Order in the Kagome Ising Magnet Dy3Mg2Sb3O14

The kagome lattice -- a two-dimensional (2D) arrangement of corner-sharing triangles -- is at the forefront of the search for exotic states generated by magnetic frustration. Such states have been observed experimentally for Heisenberg and planar spins. In contrast, frustration of Ising spins on the kagome lattice has previously been restricted to nano-fabricated systems and spin-ice materials under applied magnetic field. Here, we show that the layered Ising magnet Dy3Mg2Sb3O14 hosts an emergent order predicted theoretically for individual kagome layers of in-plane Ising spins. Neutron-scattering and bulk thermomagnetic measurements, supported by Monte Carlo simulations, reveal a phase transition at T* = 0.3 K from a disordered spin-ice like regime to an "emergent charge ordered" state in which emergent charge degrees of freedom exhibit three-dimensional order while spins remain partially disordered. Our results establish Dy3Mg2Sb3O14 as a tuneable system to study interacting emergent charges arising from kagome Ising frustration.

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arXiv2015

Raman study of magnetic excitations and magneto-elastic coupling in alpha-SrCr2O4

Using Raman spectroscopy, we investigate the lattice phonons, magnetic excitations, and magneto-elastic coupling in the distorted triangular-lattice Heisenberg antiferromagnet alpha-SrCr2O4, which develops helical magnetic order below 43 K. Temperature dependent phonon spectra are compared to predictions from density functional theory calculations which allows us to assign the observed modes and identify weak effects arising from coupled lattice and magnetic degrees of freedom. Raman scattering associated with two-magnon excitations is observed at 20 meV and 40 meV. These energies are in general agreement with our ab-initio calculations of exchange interactions and earlier theoretical predictions of the two-magnon Raman response of triangular-lattice antiferromagnets. The temperature dependence of the two-magnon excitations indicates that spin correlations persist well above the Néel temperature.

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