arXiv subjects

D. Mandrus

Publications and source records attributed to D. Mandrus.

At least 19 recordsLinked to original sources

arXiv2026

Magnetic order and excitations in Ce$_3$TiBi$_5$ and Ce$_3$ZrBi$_5$

The R3MBi5 rare-earth intermetallics (R = rare earth, M = Ti, Zr, Sc) provide a versatile platform to explore how Kondo hybridization, RKKY exchange, magnetic frustration, and broken inversion symmetry may cooperate to generate unusual magnetic behavior. We present a comprehensive neutron scattering investigation of the magnetic structure, crystal electric field (CEF), and low-energy excitations in the locally noncentrosymmetric Kondo-lattice compounds Ce3TiBi5 and Ce3ZrBi5. Powder and single-crystal neutron diffraction reveals incommensurate cycloidal antiferromagnetic order in Ce3TiBi5 with propagation vector k = (0, 0, 0.388) and a reduced ordered moment of m = 0.53(3)$\mu_{B}$. Ce3ZrBi5 exhibits a qualitatively similar magnetic diffraction profile, with k $\simeq$ (0, 0, 0.37). Inelastic neutron scattering measurements resolve two clear, well-separated CEF excitations in both compounds with nearly the same profile, confirming a well-isolated Kramers doublet ground state. At low energies, a broad, quasi-elastic magnetic response is observed at T $\simeq$ TN, whose momentum-dependence is inconsistent with that expected from conventional collective excitations of localized moments. This discrepancy, along with a Kondo temperature estimate TK ~ 3--5 K -- comparable to TN -- indicates sizable Kondo hybridization, which accounts for the moment reduction and the spiral magnetic order that appears to involve the magnetic hard direction. Our results place these compounds in a regime where local inversion symmetry breaking, anisotropic CEF effects, and competing Kondo and RKKY interactions collectively give rise to unconventional magnetic order.

cond-mat.str-el↗

arXiv2025

Formation of Frustrated Charge Density Waves in Kagome Metal LuNb$_6$Sn$_6$

The charge density wave (CDW), a translational symmetry breaking electronic liquid, plays a pivotal role in correlated quantum materials, such as high-T$_c$ superconductors and topological semimetals. Recently, CDWs that possibly intertwine with superconductivity and magnetism are observed in various kagome metals. However, the nature of CDWs and the role of the Fermi surface (FS) topology in these materials remain an unresolved challenge. In this letter, we reveal the formation of CDWs in the newly discovered kagome metal LuNb$_6$Sn$_6$. We observe a precursor CDW correlation that features a "yield sign"-like hollow triangle diffuse scattering pattern and nearly complete softening of a flat optical phonon band near Q$_H$=(1/3, 1/3, 1/2). The scattering intensity of the precursor CDW displays divergent behavior as decreasing temperature until T$_{CDW}$=70 K, where a competing CDW at Q$_{CDW}$=(1/3, 1/3, 1/3) emerges. Using scanning tunneling microscopy/spectroscopy, we image the frustrated CDW patterns that show a short phase coherence length about ~20 nm in real space. Combined with first principles calculations, our observations support frustrated lattice interactions that are modulated by the FS topology. These results shed light on the interplay between FS and CDW in quantum materials with nearly degenerate structural deformation patterns.

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arXiv2022

Spin sensitive transport in RuCl_3/Pt heterostructures: revealing a field-transverse spin anisotropy in a spin liquid candidate

Alpha-phase (a-) RuCl_3 has emerged as a possible candidate for a quantum spin liquid (QSL) that promises exotic quasi-particles relevant for fault-tolerant quantum computation. Here, we report spin-sensitive transport measurements using a proximal spin Hall metal -- platinum (Pt) -- to probe magnetic moments in the insulator a-RuCl_3. We observe a spin Hall magnetoresistance (SMR) where both the transverse and longitudinal resistivities of a-RuCl_3/Pt exhibit oscillations as functions of the angle between the in-plane magnetic field and the current, arising from the interplay between the spin Hall effect in Pt and local magnetic moments in a-RuCl3. The oscillations are observed from 1.5 T to 18 T, spanning the range of magnetic fields where zig-zag antiferromagnetic phase, the putative QSL phase, and the partially field-polarized states are reported in a-RuCl_3. The phase of the SMR oscillations suggest that the local moments, regardless of static or fluctuating, in a-RuCl_3 develop an anisotropy with an in-plane quantization axis that aligns largely transverse to the magnetic field for all fields above 1.5 T. Temperature dependance of the SMR revealed that the spin anisotropy has a similar energy scale to reported QSL signatures in a-RuCl_3. The coupling between the spin states within a-RuCl_3 and Pt demonstrated in our experiment opens a transport route to exploring exotic spin phases and device functionalities of QSL materials.

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arXiv2022

Spin dynamics in the skyrmion-host lacunar spinel GaV4S8

In the lacunar spinel GaV4S8, the interplay of spin, charge, and orbital degrees of freedom produces a rich phase diagram that includes an unusual Neel-type skyrmion phase composed of molecular spins. To provide insight into the interactions underlying this complex phase diagram, we study the spin excitations in GaV4S8 through inelastic neutron scattering measurements on polycrystalline and single-crystal samples. Using linear spin-wave theory, we describe the spin-wave excitations using a model where V4 clusters decorate an FCC lattice. The effective cluster model includes a ferromagnetic interaction and a weaker antisymmetric Dzyaloshinskii-Moriya (DM) interaction between the neighboring molecular spins. Our work clarifies the spin interactions in GaV4S8 and supports the picture of interacting molecular clusters.

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arXiv2021

Evidence of a Phonon Hall Effect in the Kitaev Spin Liquid Candidate $\alpha$-RuCl$_3$

The material $\alpha$-RuCl$_3$ has been the subject of intense scrutiny as a potential Kitaev quantum spin liquid, predicted to display Majorana fermions as low energy excitations. In practice, $\alpha$-RuCl$_3$ undergoes a transition to a state with antiferromagnetic order below a temperature $T_{\rm N}$ $\approx$ 7 K, but this order can be suppressed by applying an external in-plane magnetic field of $H_\parallel$ = 7 T. Whether a quantum spin liquid phase exists just above that field is still an open question, but the reported observation of a quantized thermal Hall conductivity at $H_\parallel$ $>$ 7 T by Kasahara and co-workers $\big[$Kasahara ${\it et \ al}$., Nature ${\bf 559}$, 227 (2018)$\big]$ has been interpreted as evidence of itinerant Majorana fermions in the Kitaev quantum spin liquid state. In this study, we re-examine the origin of the thermal Hall conductivity $\kappa_{\rm xy}$ in $\alpha$-RuCl$_3$. Our measurements of $\kappa_{\rm xy}$($T$) on several different crystals yield a temperature dependence very similar to that of the phonon-dominated longitudinal thermal conductivity $\kappa_{\rm xx}$($T$), for which the natural explanation is that $\kappa_{\rm xy}$ is also mostly carried by phonons. Upon cooling, $\kappa_{\rm xx}$ peaks at $T \simeq$ 20 K, then drops until $T_{\rm N}$, whereupon it suddenly increases again. The abrupt increase below $T_{\rm N}$ is attributed to a sudden reduction in the scattering of phonons by low-energy spin fluctuations as these become partially gapped when the system orders. The fact that $\kappa_{\rm xy}$ also increases suddenly below $T_{\rm N}$ is strong evidence that the thermal Hall effect in $\alpha$-RuCl$_3$ is also carried predominantly by phonons. This implies that any quantized signal from Majorana edge modes would have to come on top of a sizable -- and sample-dependent -- phonon background.

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arXiv2021

Giant Phonon Anomalies in the Proximate Kitaev Quantum Spin Liquid $α$-RuCl$_3$

The Kitaev quantum spin liquid epitomizes an entangled topological state, for which two flavors of fractionalized low-energy excitations are predicted: the itinerant Majorana fermion and the Z2 gauge flux. Detection of these excitations remains challenging, because of their fractional quantum numbers and non-locality. It was proposed recently that fingerprints of fractional excitations are encoded in the phonon spectra of Kitaev quantum spin liquids through a novel fractional-excitation-phonon coupling. Here, we uncover this effect in $α$-RuCl3 using inelastic X-ray scattering with meV resolution. At high temperature, we discover interlaced optical phonons intercepting a transverse acoustic phonon between 3 and 7 meV. Upon decreasing temperature, the optical phonons display a large intensity enhancement near the Kitaev energy, JK~8 meV, that coincides with a giant acoustic phonon softening near the Z2 gauge flux energy scale. This fractional excitation induced phonon anomalies uncover the key ingredient of the quantum thermal Hall effect in $α$-RuCl3 and demonstrates a proof-of-principle method to detect fractional excitations in topological quantum materials.

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arXiv2020

Low-Temperature 2D/2D Ohmic Contacts in WSe$_2$ Field-Effect Transistors as a Platform for the 2D Metal-Insulator Transition

We report the fabrication of hexagonal-boron-nitride (hBN) encapsulated multi-terminal WSe$_2$ Hall bars with 2D/2D low-temperature Ohmic contacts as a platform for investigating the two-dimensional (2D) metal-insulator transition. We demonstrate that the WSe$_2$ devices exhibit Ohmic behavior down to 0.25 K and at low enough excitation voltages to avoid current-heating effects. Additionally, the high-quality hBN-encapsulated WSe$_2$ devices in ideal Hall-bar geometry enable us to accurately determine the carrier density. Measurements of the temperature ($T$) and density ($n_s$) dependence of the conductivity $σ(T,n_s)$ demonstrate scaling behavior consistent with a metal-insulator quantum phase transition driven by electron-electron interactions, but where disorder-induced local magnetic moments are also present. Our findings pave the way for further studies of the fundamental quantum mechanical properties of 2D transition metal dichalcogenides using the same contact engineering.

cond-mat.mes-hall↗

arXiv2020

Magnetic exchange interactions in the van der Waals layered antiferromagnet MnPSe3

Two-dimensional van der Waals compounds with magnetic ions on a honeycomb lattice are hosts to a variety of exotic behavior. The magnetic interactions in one such compound, MnPSe$_3$, are investigated with elastic and inelastic neutron scattering. Magnetic excitations are observed in the magnetically ordered regime and persist to temperatures well above the ordering temperature, $\rm T_N$ = 74 K, consistent with low dimensional magnetic interactions. The inelastic neutron scattering results allow a model spin Hamiltonian to be presented that includes dominant intralayer interactions of $J_{1ab}$=0.45 meV, $J_{2ab}$=0.03 meV, $J_{3ab}$=0.19 meV, and appreciable interlayer interactions of $J_c$=0.031(5) meV. No evidence for anisotropy in the form of a spin-gap is observed in the data collected. The measurements on MnPSe$_3$ are contrasted with those on MnPS$_3$ and reveal a large increase in the interlayer exchange interactions in MnPSe$_3$, despite the quasi-2D magnetic behavior.

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arXiv2020

A continuous metal-insulator transition driven by spin correlations

Metal-insulator transitions involve a mix of charge, spin, and structural degrees of freedom, and when strongly-correlated, can underlay the emergence of exotic quantum states. Mott insulators induced by the opening of a Coulomb gap are an important and well-recognized class of transitions, but insulators purely driven by spin correlations are much less common, as the reduced energy scale often invites competition from other degrees of freedom. Here we demonstrate a clean example of a spin-correlation-driven metal-insulator transition in the all-in-all-out pyrochlore antiferromagnet Cd2Os2O7, where the lattice symmetry is fully preserved by the antiferromagnetism. After the antisymmetric linear magnetoresistance from conductive, ferromagnetic domain walls is carefully removed experimentally, the Hall coefficient of the bulk reveals four Fermi surfaces, two of electron type and two of hole type, sequentially departing the Fermi level with decreasing temperature below the Néel temperature, T_N. Contrary to the common belief of concurrent magnetic and metal-insulator transitions in Cd2Os2O7, the charge gap of a continuous metal-insulator transition opens only at T~10K, well below T_N=227K. The insulating mechanism resolved by the Hall coefficient parallels the Slater picture, but without a folded Brillouin zone, and contrasts sharply with the behavior of Mott insulators and spin density waves, where the electronic gap opens above and at T_N, respectively.

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arXiv2020

Magnetic structure and exchange interactions in the layered semiconductor CrPS4

Compounds with two-dimensional (2D) layers of magnetic ions weakly connected by van der Waals bonding offer routes to enhance quantum behavior, stimulating both fundamental and applied interest. CrPS4 is one such magnetic van der Waals material, however, it has undergone only limited investigation. Here we present a comprehensive series of neutron scattering measurements to determine the magnetic structure and exchange interactions. The observed magnetic excitations allow a high degree of constraint on the model parameters not normally associated with measurements on a powder sample. The results demonstrate the 2D nature of the magnetic interactions, while also revealing the importance of interactions along 1D chains within the layers. The subtle role of competing interactions is observed, which manifest in a non-trivial magnetic transition and a tunable magnetic structure in a small applied magnetic field through a spin-flop transition. Our results on the bulk compound provide insights that can be applied to an understanding of the behavior of reduced layer CrPS4.

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arXiv2020

Robust cycloid crossover driven by anisotropy in the skyrmion host GaV$_\mathbf{4}$S$_\mathbf{8}$

We report on the anomalous magnetization dynamics of the cycloidally-modulated spin textures under the influence of uniaxial anisotropy in multiferroic $\mathrm{GaV_4S_8}$. The temperature and field dependence of the linear ac susceptibility [$χ_{1ω}^{\prime}(T,H)$], ac magnetic loss [$χ_{1ω}^{\prime\prime}(T,H)$], and nonlinear ac magnetic response [$M_{3ω}(T,H)$] are examined across the magnetic phase diagram in the frequency range $f = 10-10000$ Hz. According to recent theory, skyrmion vortices under axial crystal symmetry are confined along specific orientations, resulting in enhanced robustness against oblique magnetic fields and altered spin dynamics. We characterize the magnetic response of each spin texture and find that the dynamic rigidity of the Néel skyrmion lattice appears enhanced compared to Bloch-type skyrmions in cubic systems, even in the multidomain state. Anomalous $M_{3ω}$ and strong dissipation emerge over the same phase regime where strong variations in the cycloid pitch were observed on lowering temperature in recent small-angle neutron scattering experiments [White et al., Phys. Rev. B 97, 020401(R) (2018)]. Here, we show that strong anisotropy also drives an extended crossover of the zero-field cycloid texture in $\mathrm{GaV_4S_8}$. The frequency dependence of these dynamic signatures is consistent with that of a robust anharmonic spin texture exhibiting a correlated domain arrangement. The results underpin the essential role of magnetic anisotropy in enhancing the rigidity of topological spin textures for diverse applications.

cond-mat.mes-hall↗

arXiv2020

Van Hove singularity in the magnon spectrum of the antiferromagnetic quantum honeycomb lattice

The magnetic excitation spectrum of the quantum magnet YbCl$_3$ is studied with inelastic neutron scattering. The spectrum exhibits an unusually sharp feature within a broad continuum, as well as conventional spin waves. By including both transverse and longitudinal channels of the neutron response, linear spin wave theory with a single Heisenberg interaction on the honeycomb lattice reproduces all of the key features in the spectrum. In particular, the broad continuum corresponds to a two-magnon contribution from the longitudinal channel, while the sharp feature within this continuum is identified as a Van Hove singularity in the joint density of states, which indicates the two-dimensional nature of the two-magnon continuum. We term these singularities magneto-caustic features in analogy with caustic features in ray optics where focused envelopes of light are generated when light passes through or reflects from curved or distorted surfaces. The experimental demonstration of a sharp Van Hove singularity in a two-magnon continuum is important because analogous features in potential two-spinon continua could distinguish quantum spin liquids from merely disordered systems. These results establish YbCl$_3$ as a nearly ideal two-dimensional honeycomb lattice material hosting strong quantum effects in the unfrustrated limit.

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arXiv2020

Spin and orbital dynamics through the metal-to-insulator transition in Cd$_2$Os$_2$O$_7$ probed with high-resolution RIXS

High-resolution resonant inelastic x-ray scattering (RIXS) measurements ($Δ$E = 46 meV) have been performed on Cd$_2$Os$_2$O$_7$ through the metal-to-insulator transition (MIT). A magnetic excitation at 125 meV evolves continuously through the MIT, in agreement with recent Raman scattering results, and provides further confirmation for an all-in, all-out magnetic ground state. Asymmetry of this feature is likely a result of coupling between the electronic and magnetic degrees of freedom. We also observe a broad continuum of interband excitations centered at 0.3 eV energy loss. This is indicative of significant hybridization between Os 5$d$ and O 2$p$ states, and concurrent itinerant nature of the system. In turn, this suggests a possible break down of the free-ion model for Cd$_2$Os$_2$O$_7$.

cond-mat.str-el↗

arXiv2019

Polarization-resolved Raman spectroscopy of α-RuCl3 and evidence of room temperature two-dimensional magnetic scattering

Polarization-resolved Raman spectroscopy was performed and analyzed from large, high quality, mono-domain single crystal of α-RuCl3, a proximate Kitaev quantum spin liquid. Spectra were collected with laser polarizations parallel and perpendicular to the honeycomb plane. Pairs of nearly degenerate phonons were discovered and show either a 4-fold or 2-fold polarization angle dependence in their Raman intensity, thereby providing evidence to definitively assign the bulk crystal point group as C2h. The low frequency continuum that is often attributed to scattering from pairs of Majorana fermions was also examined and found to disappear when the laser excitation and scattered photon polarizations were perpendicular to the honeycomb plane. This disappearance, along with the behavior of the phonon spectrum in the same polarization configuration, strongly suggests that the scattering continuum is 2-dimensional. We argue that this scattering continuum originates from the Kitaev magnetic interactions that survives up to room temperature, a scale larger than the bare Kitaev exchange energy of approximately 50 K.

cond-mat.str-el↗

arXiv2019

51V-NMR study on the S=1/2 square lattice antiferromagnet K2V3O8

Static and dynamic properties of the quasi-two-dimensional antiferromagnet K$_2$V$_3$O$_8$ have been investigated by $^{51}$V-NMR experiments on nonmagnetic V$^{5+}$ sites. Above the structural transition temperature $T_{\rm{S}}$ = 115 K, NMR spectra are fully compatible with the $P4bm$ space group symmetry. The formation of superstructure below $T_{\rm{S}}$ causes splitting of the NMR lines, which get broadened at lower temperatures so that individual peaks are not well resolved. Evolution of NMR spectra with magnetic field along $c$-axis below the magnetic transition temperature $T_{\rm{N}} \sim 4$ K is qualitatively consistent with a simple Néel order and a spin flop transition. However, broad feature of the spectra does not rule out possible incommensurate spin structure. The spin-lattice relaxation rate $1/T_1$ below $T_{\rm{N}}$ shows huge enhancement for a certain range of magnetic field, which is independent of temperature and attributed to cross relaxation due to anomalously large nuclear spin-spin coupling between V$^{5+}$ and magnetic V$^{4+}$ sites. The results indicate strong gapless spin fluctuations, which could arise from incommesurate orders or complex spin textures.

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arXiv2019

Odd-parity linear magnetoresistance and the planar Hall effect

The phenomena of odd-parity magnetoresistance and the planar Hall effect are deeply entwined with ferromagnetism. The intrinsic magnetization of the ordered state permits these unusual and rarely observed manifestations of Onsager's theorem when time reversal symmetry is broken at zero applied field. Here we study two classes of ferromagnetic materials, rare-earth magnets with high intrinsic coercivity and antiferromagnetic pyrochlores with strongly-pinned ferromagnetic layers at domain walls, which both exhibit odd-parity magnetoresistive behavior. The peculiar angular variation of the response with respect to the relative alignments of the magnetization, magnetic field, and current reveal the two underlying microscopic mechanisms: spin-polarization-dependent scattering of a Zeeman-shifted Fermi surface and magnetoresistance driven by the anomalous velocity physics usually associated with the anomalous Hall effect.

cond-mat.str-el↗

arXiv2018

Physical properties of the trigonal binary compound Nd$_2$O$_3$

We have studied the physical properties of Nd$_2$O$_3$ with neutron diffraction, inelastic neutron scattering, heat capacity, and magnetic susceptibility measurements. Nd$_2$O$_3$ crystallizes in a trigonal structure, with Nd$^{3+}$ ions surrounded by cages of 7 oxygen anions. The crystal field spectrum consists of four excitations spanning the energy range 3-60 meV. The refined eigenfunctions indicate XY-spins in the $ab$ plane. The Curie-Weiss temperature of $θ_{CW}=-23.7(1)$ K was determined from magnetic susceptibility measurements. Heat capacity measurements show a sharp peak at 550 mK and a broader feature centered near 1.5 K. Neutron diffraction measurements show that the 550 mK transition corresponds to long-range anti-ferromagnetic order implying a frustration index of $θ_{CW}/T_N\approx43$. These results indicate that Nd$_2$O$_3$ is a structurally and chemically simple model system for frustration caused by competing interactions with moments with predominate XY anisotropy.

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arXiv2018

Extended exchange interactions stabilize long-period magnetic structures in Cr$_{1/3}$NbS$_2$

The topologically-protected, chiral soliton lattice is a unique state of matter offering intriguing functionality and it may serve as a robust platform for storing and transporting information in future spintronics devices. While the monoaxial chiral magnet Cr$_{1/3}$NbS$_2$ is known to host this exotic state in an applied magnetic field, its detailed microscopic origin has remained a matter of debate. Here we work towards addressing this open question by measuring the spin wave spectrum of Cr$_{1/3}$NbS$_2$ over the entire Brillouin zone with inelastic neutron scattering. The well-defined spin wave modes allow us to determine the values of several microscopic interactions for this system. The experimental data is well-explained by a Heisenberg Hamiltonian with exchange constants up to third nearest neighbor and an easy plane magnetocrystalline anisotropy term. Our work shows that both the second and third nearest neighbor exchange interactions contribute to the formation of the helimagnetic and chiral soliton lattice states in this robust three-dimensional magnet.

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