arXiv subjects

D. G. Mandrus

Publications and source records attributed to D. G. Mandrus.

At least 19 recordsLinked to original sources

arXiv2026

Magnetic Field Dependence of the Spin Fluctuations in CeCu$_{5.8}$Ag$_{0.2}$

Quantum phase transitions are among the most intriguing phenomena that can occur when the electronic ground state of correlated metals are tuned by external parameters such as pressure, magnetic field or chemical substitution. Such transitions between distinct states of matter are driven by quantum fluctuations, and can give rise to macroscopically coherent phases that are at the forefront of condensed matter research. However, the nature of the critical fluctuations, and thus the fundamental physics controlling many quantum phase transitions, remain poorly understood in numerous strongly correlated metals. Here we study the model material CeCu$_{5.8}$Ag$_{0.2}$ to gain insight into the implications of critical fluctuations originating from different regions in reciprocal space. By employing an external magnetic field along the crystallographic $a$- and $c$-axis as auxiliary tuning parameter we observe a pronounced anisotropy in the suppression of the quantum critical fluctuations, reflecting the spin anisotropy of the long-range ordered ground state at larger silver concentration. Coupled with the temperature dependence of the quantum critical fluctuations, these results suggest that the quantum phase transition in CeCu$_{5.8}$Ag$_{0.2}$ is driven by three-dimensional spin-density wave fluctuations.

cond-mat.str-el↗

arXiv2025

Strain-induced multiferroicity in Cr1/3NbS2

Multiferroic materials, in which electric polarization and magnetic order coexist and couple, offer rich opportunities for both fundamental discovery and technology. However, multiferroicity remains rare due to conflicting electronic requirements for ferroelectricity and magnetism. One route to circumvent this challenge is to exploit the noncollinear ordering of spin cycloids, whose symmetry permits the emergence of polar order. In this work, we introduce another pathway to multiferroic order in which strain generates polarization in materials that host nonpolar spin spirals. To demonstrate this phenomenon, we chose the spin spiral in the well-studied helimagnet Cr1/3NbS2. To detect the induced polarization, we introduce the technique of magnetoelectric birefringence (MEB), an optical probe that enables spatially-resolved and unambiguous detection of polar order. By combining MEB imaging with strain engineering, we confirm the onset of a polar vector at the magnetic transition, establishing strained Cr1/3NbS2 as a type-II multiferroic.

cond-mat.mtrl-sci↗

arXiv2023

Imaging exciton-polariton transport in MoSe2 waveguides

The exciton polariton (EP), a half-light and half-matter quasiparticle, is potentially an important element for future photonic and quantum technologies. It provides both strong light-matter interactions and long-distance propagation that is necessary for applications associated with energy or information transfer. Recently, strongly-coupled cavity EPs at room temperature have been demonstrated in van der Waals (vdW) materials due to their strongly-bound excitons. Here we report a nano-optical imaging study of waveguide EPs in MoSe2, a prototypical vdW semiconductor. The measured propagation length of the EPs is sensitive to the excitation photon energy and reaches over 12 μm. The polariton wavelength can be conveniently altered from 600 nm down to 300 nm by controlling the waveguide thickness. Furthermore, we found an intriguing mode back-bending dispersion close to the exciton resonance. The observed EPs in vdW semiconductors could be useful in future nanophotonic circuits operating in the near-infrared to visible spectral regions.

physics.optics↗

arXiv2022

Nanometric modulations of the magnetic structure of the element Nd

The rare earth neodymium arguably exhibits the most complex magnetic ordering and series of magnetic phase transitions of the elements. Here we report the results of small-angle neutron scattering (SANS) measurements as a function of temperature and applied magnetic field to study magnetic correlations on nanometer length scales in Nd. The SANS measurements reveal the presence of previously unreported modulation vectors characterizing the ordered spin configuration which exhibit changes in magnitude and direction that are phase dependent. Between 5.9 and 7.6 K the additional modulation vector has a magnitude $Q$ =0.12 Å$^{-1}$ and is primarily due to order of the Nd layers which contain a center of inversion. In this region of the phase diagram, the SANS measurements also identify a phase boundary at $\approx$1 T. An important feature of these modulation vectors is that they indicate the presence of nanometer length scale spin textures which are likely stabilized by frustrated Ruderman-Kittel-Kasuya-Yosida (RKKY) interactions rather than a Dzyaloshinskii-Moriya (DM) exchange interaction.

cond-mat.str-el↗

arXiv2021

Disentangling Electronic, Lattice and Spin Dynamics in the Chiral Helimagnet Cr1/3NbS2

We investigate the static and ultrafast magneto-optical response of the hexagonal chiral helimagnet $Cr_{1/3}NbS_{2}$ above and below the helimagnetic ordering temperature. The presence of a magnetic easy plane contained within the crystallographic ab-plane is confirmed, while degenerate optical pump-probe experiments reveal significant differences in the dynamic between the parent, $NbS_{2}$, and Cr-intercalated compounds. Time resolved magneto-optical Kerr effect measurements show a two-step demagnetization process, where an initial, sub-ps relaxation and subsequent buildup ($τ> 50$ ps) in the demagnetization dynamic scale similarly with increasing pump fluence. Despite theoretical evidence for partial gapping of the minority spin channel, suggestive of possible half metallicity in $Cr_{1/3}NbS_{2}$, such a long demagnetization dynamic likely results from spin lattice-relaxation as opposed to minority state blocking. However, comparison of the two-step demagnetization process in $Cr_{1/3}NbS_{2}$ with other 3d intercalated transition metal dichalcogenides reveals a behavior that is unexpected from conventional spin-lattice relaxation, and may be attributed to the complicated interaction of local moments with itinerant electrons in this material system.

cond-mat.mtrl-sci↗

arXiv2021

Field-induced intermediate phase in $α$-RuCl$_3$: Non-coplanar order, phase diagram, and proximate spin liquid

Frustrated magnets with strong spin-orbit coupling promise to host topological states of matter, with fractionalized excitations and emergent gauge fields. Kitaev's proposal for a honeycomb-lattice Majorana spin liquid has triggered an intense search for experimental realizations, with bond-dependent Ising interaction being the essential building block. A prime candidate is $α$-RuCl$_3$ whose phase diagram in a magnetic field is, however, not understood to date. Here we present conclusive experimental evidence for a novel field-induced ordered phase in $α$-RuCl$_3$, sandwiched between the zigzag and quantum disordered phases at low and high fields, respectively. We provide a detailed theoretical study of the relevant effective spin model which we show to display a field-induced intermediate phase as well. We fully characterize the intermediate phase within this model, including its complex spin structure, and pinpoint the parameters relevant to $α$-RuCl$_3$ based on the experimentally observed critical fields. Most importantly, our study connects the physics of $α$-RuCl$_3$ to that of the Kitaev-$Γ$ model, which displays a quantum spin liquid phase in zero field, and hence reveals the spin liquid whose signatures have been detected in a variety of dynamical probes of $α$-RuCl$_3$.

cond-mat.str-el↗

arXiv2021

Imaging the Néel vector switching in the monolayer antiferromagnet MnPSe$_3$ with strain-controlled Ising order

The family of monolayer two-dimensional (2D) materials hosts a wide range of interesting phenomena, including superconductivity, charge density waves, topological states and ferromagnetism, but direct evidence for antiferromagnetism in the monolayer has been lacking. Nevertheless, antiferromagnets have attracted enormous interest recently in spintronics due to the absence of stray fields and their terahertz resonant frequency. Despite the great advantages of antiferromagnetic spintronics, controlling and detecting Néel vectors have been limited in bulk materials. In this work, we developed a sensitive second harmonic generation (SHG) microscope and detected long-range Néel antiferromagnetic (AFM) order and Néel vector switching down to the monolayer in MnPSe$_3$. Temperature-dependent SHG measurement in repetitive thermal cooling surprisingly collapses into two curves, which correspond to the switching of an Ising type Néel vector reversed by the time-reversal operation, instead of a six-state clock ground state expected from the threefold rotation symmetry in the structure. We imaged the spatial distribution of the Néel vectors across samples and rotated them by an arbitrary angle irrespective of the lattice in the sample plane by applying strain. By studying both a Landau theory and a microscopic model that couples strain to nearest-neighbor exchange, we conclude that the phase transition of the XY model in the presence of strain falls into the Ising universality class instead of the XY one, which could explain the extreme strain tunability. Finally, we found that the 180° AFM domain walls are highly mobile down to the monolayer after thermal cycles, paving the way for future control of the antiferromagnetic domains by strain or external fields on demand for ultra-compact 2D AFM terahertz spintronics.

cond-mat.mtrl-sci↗

arXiv2020

The nature of ferromagnetism in the chiral helimagnet $Cr_{1/3}NbS_{2}$

The chiral helimagnet, $Cr_{1/3}NbS_{2}$, hosts exotic spin textures, whose influence on the magneto-transport properties, make this material an ideal candidate for future spintronic applications. To date, the interplay between macroscopic magnetic and transport degrees of freedom is believed to result from a reduction in carrier scattering following spin order. Here, we present electronic structure measurements through the helimagnetic transition temperature, $T_{C}$ that challenges this view by showing a Fermi surface comprised of strongly hybridized Nb- and Cr- derived electronic states, and spectral weight in proximity to the Fermi level to anomalously increases as temperature is lowered below $T_{C}$. These findings are rationalized on the basis of first principle, density functional theory calculations, which reveal a large nearest-neighbor exchange energy, suggesting the interaction between local spin moments and hybridized Nb- and Cr- derived itinerant states to go beyond the perturbative interaction of Ruderman-Kittel-Kasuya-Yosida, suggesting instead a mechanism rooted in a Hund's exchange interaction.

cond-mat.mtrl-sci↗

arXiv2020

Nature of Magnetic Excitations in the High-Field Phase of $α$-RuCl$_3$

We present comprehensive electron spin resonance (ESR) studies of in-plane oriented single crystals of $α$-RuCl$_3$, a quasi-two-dimensional material with honeycomb structure, focusing on its high-field spin dynamics. The measurements were performed in magnetic fields up to 16 T, applied along the [110] and [100] directions. Several ESR modes were detected. Combining our findings with recent inelastic neutron- and Raman-scattering data, we identify most of the observed excitations. Most importantly, we show that the low-temperature ESR response beyond the boundary of the magnetically ordered region is dominated by single- and two-particle processes with magnons as elementary excitations. The peculiarities of the excitation spectrum in the vicinity of the critical field are discussed.

cond-mat.str-el↗

arXiv2020

Field-induced phase transitions of the Kitaev material $α$-RuCl$_3$ probed by thermal expansion and magnetostriction

High-resolution thermal expansion and magnetostriction measurements were performed on single crystals of $α$-RuCl$_3$ in magnetic fields applied parallel to the Ru-Ru bonds. The length changes were measured in the direction perpendicular to the honeycomb planes. Our data show clear thermodynamic characteristics for the field-induced phase transition at the critical field $μ_0H_{c1} = 7.8(2)$ T where the antiferromagnetic zigzag order is suppressed. At higher fields, a kink in the magnetostriction coefficient signals an additional phase transition around $μ_0H_{c2} \approx 11$ T. The extracted Grüneisen parameter shows typical hallmarks for quantum criticality near $H_{c1}$, but also displays anomalous behavior above $H_{c1}$. We compare our experimental data with linear spin-wave calculations employing a minimal Kitaev-Heisenberg model in the semiclassical limit. Most of the salient features are in agreement with each other, however, the peculiar features in the high-field region above $H_{c1}$ cannot be accounted for in our modelling and hence suggest a genuine quantum nature. We construct a phase diagram for $α$-RuCl$_3$ showing two low-temperature transitions induced by an in-plane field along the Ru-Ru bonds.

cond-mat.str-el↗

arXiv2019

Evidence for charge transfer and proximate magnetism in graphene/a-RuCl_3 heterostructures

We report a study of electronic transport in van der Waals heterostructures composed of flakes of the antiferromagnetic Mott insulator a-RuCl_3 placed on top of monolayer graphene Hall bars. While the zero-field transport shows a strong resemblance to that of isolated graphene, we find a consistently $p$-type Hall effect suggestive of multiband conduction, along with a non-monotonic and gate-voltage-dependent excursion of the resistivity at low temperatures that is reminiscent of transport in the presence of a magnetic phase transition. We interpret these data as evidence for charge transfer from graphene to a-RuCl_3 in an inhomogeneous device yielding both highly- and lightly-doped regions of graphene, while the latter shows a particular sensitivity to magnetism in the a-RuCl_3. Thus proximity to graphene is a means to access magnetic properties of thin layers of magnetic insulators.

cond-mat.str-el↗

arXiv2018

Pressure-induced dimerization and valence bond crystal formation in the Kitaev-Heisenberg magnet alpha-RuCl3

Magnetization and high-resolution x-ray diffraction measurements of the Kitaev-Heisenberg material alpha-RuCl3 reveal a pressure-induced crystallographic and magnetic phase transition at a hydrostatic pressure of p=0.2 GPa. This structural transition into a triclinic phase is characterized by a very strong dimerization of the Ru-Ru bonds, accompanied by a collapse of the magnetic susceptibility. Ab initio quantum-chemistry calculations disclose a pressure-induced enhancement of the direct 4d-4d bonding on particular Ru-Ru links, causing a sharp increase of the antiferromagnetic exchange interactions. These combined experimental and computational data show that the Kitaev spin liquid phase in alpha-RuCl3 strongly competes with the crystallization of spin singlets into a valence bond solid.

cond-mat.str-el↗

arXiv2018

Evidence of an improper displacive phase transition in Cd$_2$Re$_2$O$_7$ via time-resolved coherent phonon spectroscopy

We have used a combination of ultrafast coherent phonon spectroscopy, ultrafast thermometry, and time-dependent Landau theory to study the inversion symmetry breaking phase transition at $T_c = 200$ K in the strongly spin-orbit coupled correlated metal Cd$_2$Re$_2$O$_7$. We establish that the structural distortion at $T_c$ is a secondary effect through the absence of any softening of its associated phonon mode, which supports a purely electronically driven mechanism. However, the phonon lifetime exhibits an anomalously strong temperature dependence that decreases linearly to zero near $T_c$. We show that this behavior naturally explains the spurious appearance of phonon softening in previous Raman spectroscopy experiments and should be a prevalent feature of correlated electron systems with linearly coupled order parameters.

cond-mat.str-el↗

arXiv2017

Unconventional spin dynamics in the honeycomb-lattice material $α$-RuCl$_3$: high-field ESR studies

We present high-field electron spin resonance (ESR) studies of the honeycomb-lattice material $α$-RuCl$_3$, a prime candidate to exhibit Kitaev physics. Two modes of antiferromagnetic resonance were detected in the zigzag ordered phase, with magnetic field applied in the $ab$ plane. A very rich excitation spectrum was observed in the field-induced quantum paramagnetic phase. The obtained data are compared with results of recent numerical calculations, strongly suggesting a very unconventional multiparticle character of the spin dynamics in $α$-RuCl$_3$. The frequency-field diagram of the lowest-energy ESR mode is found consistent with the behavior of the field-induced energy gap, revealed by thermodynamic measurements.

cond-mat.str-el↗

arXiv2017

Magnetism out of disorder in a J=0 compound Ba2YIrO6

We systematically investigate the magnetic properties and local structure of Ba2YIrO6 to demonstrate that Y and Ir lattice defects in the form of antiphase boundary or clusters of antisite disorder affect the magnetism observed in this $d^4$ compound. We compare the magnetic properties and atomic imaging of (1) a slow cooled crystal, (2) a crystal quenched from 900\degree C after growth, and (3) a crystal grown using a faster cooling rate than the slow cooled one. Atomic imaging by scanning transmission electron microscopy (STEM) shows that quenching from 900oC introduces antiphase boundary to the crystals, and a faster cooling rate during crystal growth leads to clusters of Y and Ir antisite disorder. STEM study suggests the antiphase boundary region is Ir-rich with a composition of Ba2YIrO6. The magnetic measurements show that Ba2YIrO6 crystals with clusters of antisite defects have a larger effective moment and a larger saturation moment than the slow-cooled crystals. Quenched crystals with Ir-rich antiphase boundary shows a slightly suppressed saturation moment than the slow cooled crystals, and this seems to suggest that antiphase boundary is detrimental to the moment formation. Our DFT calculations suggest magnetic condensation is unlikely as the energy to be gained from superexchange is small compared to the spin-orbit gap. However, once Y is replaced by Ir in the antisite disordered region, the picture of local non-magnetic singlets breaks down and magnetism can be induced. This is because of (a) enhanced interactions due to increased overlap of orbitals between sites, and, (b) increased number of orbitals mediating the interactions. Our work highlights the importance of lattice defects in understanding the experimentally observed magnetism in Ba2YIrO6 and other J=0 systems.

cond-mat.mtrl-sci↗

arXiv2017

Excitations in the field-induced quantum spin liquid state of alpha-RuCl3

The Kitaev model on a honeycomb lattice predicts a paradigmatic quantum spin liquid (QSL) exhibiting Majorana Fermion excitations. The insight that Kitaev physics might be realized in practice has stimulated investigations of candidate materials, recently including alpha-RuCl3. In all the systems studied to date, non-Kitaev interactions induce magnetic order at low temperature. However, in-plane magnetic fields of roughly 8 Tesla suppress the long-range magnetic order in alpha-RuCl3 raising the intriguing possibility of a field-induced QSL exhibiting non-Abelian quasiparticle excitations. Here we present inelastic neutron scattering in alpha-RuCl3 in an applied magnetic field. At a field of 8 Tesla, the spin waves characteristic of the ordered state vanish throughout the Brillouin zone. The remaining single dominant feature of the response is a broad continuum centered at the Gamma point, previously identified as a signature of fractionalized excitations. This provides compelling evidence that a field-induced QSL state has been achieved.

cond-mat.mtrl-sci↗

arXiv2017

A parity-breaking electronic nematic phase transition in the spin-orbit coupled metal Cd$_2$Re$_2$O$_7$

Strong electron interactions can drive metallic systems toward a variety of well-known symmetry-broken phases, but the instabilities of correlated metals with strong spin-orbit coupling have only recently begun to be explored. We uncovered a multipolar nematic phase of matter in the metallic pyrochlore Cd$_2$Re$_2$O$_7$ using spatially resolved second-harmonic optical anisotropy measurements. Like previously discovered electronic nematic phases, this multipolar phase spontaneously breaks rotational symmetry while preserving translational invariance. However, it has the distinguishing property of being odd under spatial inversion, which is allowed only in the presence of spin-orbit coupling. By examining the critical behavior of the multipolar nematic order parameter, we show that it drives the thermal phase transition near 200 kelvin in Cd$_2$Re$_2$O$_7$ and induces a parity-breaking lattice distortion as a secondary order.

cond-mat.str-el↗

arXiv2016

Bipolar Conduction is the Origin of the Electronic Transition in Pentatellurides: Metallic vs. Semiconducting Behavior

The pentatellurides, ZrTe5 and HfTe5 are layered compounds with one dimensional transition-metal chains that show a never understood temperature dependent transition in transport properties as well as recently discovered properties suggesting topological semimetallic behavior. Here we show that these materials are semiconductors and that the electronic transition is due to a combination of bipolar effects and different anisotropies for electrons and holes. We report magneto-transport properties for two kinds of ZrTe5 single crystals grown with the chemical vapor transport (S1) and the flux method (S2), respectively. These have distinct transport properties at zero field: the S1 displays a metallic behavior with a pronounced resistance peak and a sudden sign reversal in thermopower at approximately 130 K, consistent with previous observations of the electronic transition; in strikingly contrast, the S2 exhibits a semiconducting-like behavior at low temperatures and a positive thermopower over the whole temperature range. Refinements on the single-crystal X-ray diffraction and the energy dispersive spectroscopy analysis revealed the presence of noticeable Te-vacancies in the sample S1, confirming that the widely observed anomalous transport behaviors in pentatellurides actually take place in the Te-deficient samples. Electronic structure calculations show narrow gap semiconducting behavior, with different transport anisotropies for holes and electrons. For the degenerately doped n-type samples, our transport calculations can result in a resistivity peak and crossover in thermopower from negative to positive at temperatures close to that observed experimentally. Our present work resolves the longstanding puzzle regarding the anomalous transport behaviors of pentatellurides, and also resolves the electronic structure in favor of a semiconducting state.

cond-mat.mtrl-sci↗