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Helimagnetism from competing intra- and interchain interactions in CrBr$_2$ and CrI$_2$
Authors:
John A. Schneeloch,
Matthew B. Stone,
Zachary Morgan,
Despina Louca
Abstract:
CrBr$_2$ and CrI$_2$ are promising platforms for studying the effect of dimensionality on magnetic order, having been isolated in a 3-, 2-, and 1-dimensional form as bulk crystals, monolayers, and individual chains encapsulated in carbon nanotubes. However, the interactions that give rise to their helimagnetic order are unknown. Via inelastic neutron scattering on single crystals, we have determin…
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CrBr$_2$ and CrI$_2$ are promising platforms for studying the effect of dimensionality on magnetic order, having been isolated in a 3-, 2-, and 1-dimensional form as bulk crystals, monolayers, and individual chains encapsulated in carbon nanotubes. However, the interactions that give rise to their helimagnetic order are unknown. Via inelastic neutron scattering on single crystals, we have determined the exchange interactions of these compounds from the spin wave dispersions, finding that the helimagnetic order arises primarily from competing antiferromagnetic interactions between intrachain and interchain nearest-neighbors. Single-ion anisotropy is substantial, modulating the helical spin rotation and gapping the inelastic intensity at points of branch crossings. As temperature increases, long-range order vanishes but intralayer correlations remain detectable up to at least 50 K.
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Submitted 10 August, 2026;
originally announced August 2026.
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Exchange anisotropy-driven noncollinear magnetism and magnetic transitions in MnTiO3 ilmenite
Authors:
Srimal Rathnayaka,
Luke Daemen,
Despina Louca
Abstract:
Evidence for multiple magnetic transitions and unconventional spin exchange interactions in the ilmenite insulator MnTiO3 is provided via neutron scattering. On cooling, while G-type antiferromagnetic (AFM) order sets in first at 63 K with a k1 = (000) characteristic wave vector, a weaker second magnetic transition with k2 = (00 3/2 ) appears near 42 K, giving rise to a noncollinear structure. Int…
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Evidence for multiple magnetic transitions and unconventional spin exchange interactions in the ilmenite insulator MnTiO3 is provided via neutron scattering. On cooling, while G-type antiferromagnetic (AFM) order sets in first at 63 K with a k1 = (000) characteristic wave vector, a weaker second magnetic transition with k2 = (00 3/2 ) appears near 42 K, giving rise to a noncollinear structure. Intrinsic buckling of the honeycomb lattice along c creates bond anisotropy and a distorted crystal field that can lead to exchange paths that modulate orbital overlap and spin-orbit coupling. The inelastic spectrum is best described by magnetic exchange anisotropy that breaks the local symmetry of the honeycomb, with competing AFM Heisenberg, Dzyaloshinskii-Moriya and alternate intra-planar ferromagnetic (FM) interactions, that may yield a weakly-coupled ladder system.
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Submitted 5 March, 2026;
originally announced March 2026.
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Charge density wave and superconductivity modulated by c-axis stacking in the TaSe2 polytypes
Authors:
Kusal Dharmasiri,
Maxim Avdeev,
Despina Louca
Abstract:
The layered transition metal dichalcogenide, TaSe2, exhibits rich electronic phenomena across its polymorphs, 1T, 2H, and 3R, largely driven by differences in atomic coordination and c-axis stacking. In the 1T phase, octahedral coordination and AA stacking promote strong interlayer coupling and stabilize a commensurate charge density wave (CDW) with star-of-David clusters that set in at high tempe…
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The layered transition metal dichalcogenide, TaSe2, exhibits rich electronic phenomena across its polymorphs, 1T, 2H, and 3R, largely driven by differences in atomic coordination and c-axis stacking. In the 1T phase, octahedral coordination and AA stacking promote strong interlayer coupling and stabilize a commensurate charge density wave (CDW) with star-of-David clusters that set in at high temperatures. The 2H phase exhibits trigonal prismatic coordination with AB stacking, and hosts both incommensurate and commensurate CDW phases and weak superconductivity at very low temperatures. The 3R phase, characterized by ABC stacking and trigonal prismatic coordination, exhibits enhanced superconductivity along with CDW order, attributed to modified interlayer hybridization and reduced CDW competition. These stacking-dependent variations in interlayer coupling are critical in tuning correlated states in the dichalcogenides.
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Submitted 12 February, 2026;
originally announced February 2026.
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Tunable Electronic Interactions and Weak Antilocalization in Bulk Ge$_2$Sb$_2$Te$_{5-5x}$Se$_{5x}$ Phase Change Materials
Authors:
Nicholas Mazzucca,
Junjing Zhao,
Zhenyang Xu,
Despina Louca,
Utpal Chatterjee,
Marc Bockrath
Abstract:
Phase change materials (PCMs) are well-known for their reversible and rapid switching between crystalline and amorphous phases through thermal excitations mediated by strong electrical or laser pulses. This crystal-to-amorphous transition is accompanied by a remarkable contrast in optical and electronic properties, making PCMs useful in nonvolatile data storage applications. Here, we combine elect…
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Phase change materials (PCMs) are well-known for their reversible and rapid switching between crystalline and amorphous phases through thermal excitations mediated by strong electrical or laser pulses. This crystal-to-amorphous transition is accompanied by a remarkable contrast in optical and electronic properties, making PCMs useful in nonvolatile data storage applications. Here, we combine electrical transport and angle resolved photoemission spectroscopy (ARPES) measurements to study the electronic structure of bulk Ge$_2$Sb$_2$Te$_{5-5x}$Se$_{5x}$ (GSST) for $0\le x \le 0.8$, where $x$ represents the amount of Se substituting Te in Ge$_2$Sb$_2$Te$_5$ (GST)-- a prototypical PCM. The single-particle density of states (SDOS) derived from the integrated ARPES data displays metallic behavior for all $x$, as evidenced by the presence of a finite density of states in the vicinity of the chemical potential. Transport measurements also display clear signatures of metallic transport, consistent with the SDOS data. The temperature dependence of the resistance indicates the onset of moderate electron-electron Coulomb interaction effects at low temperatures for $x\geq 0.6$. At the same time, the magnetoresistance data shows signatures of weak antilocalization for $x\geq 0.6$. An analysis on the temperature dependence of the phase coherence length suggests that electron dephasing is primarily due to inelastic electron-electron scattering. We find that these effects are enhanced with increasing $x$, portraying GSST as a novel PCM where electronic interactions can be tuned via chemical doping.
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Submitted 23 September, 2025;
originally announced September 2025.
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Long-lived dynamics of the charge density wave in TiSe2 observed by time-resolved neutron diffraction
Authors:
K. Dharmasiri,
S. S. Philip,
D. Louca,
S. A. Chen,
M. D. Frontzek,
Z. J. Morgan,
C. Hua
Abstract:
We use time-resolved elastic neutron scattering combined with laser heating to probe the temporal evolution of periodic lattice distortions (PLD) due to the formation of a charge density wave (CDW) state in 1T-TiSe$_{2}$ under extreme non-equilibrium conditions. Below the transition temperature, the PLD is manifested as a 2x2x2 superlattice superimposed on the average Bragg structure. Following ra…
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We use time-resolved elastic neutron scattering combined with laser heating to probe the temporal evolution of periodic lattice distortions (PLD) due to the formation of a charge density wave (CDW) state in 1T-TiSe$_{2}$ under extreme non-equilibrium conditions. Below the transition temperature, the PLD is manifested as a 2x2x2 superlattice superimposed on the average Bragg structure. Following rapid energy deposition with the laser, kinetic bottlenecks lead to a separation of timescales between the superlattice and the underlying lattice response. The superlattice melts on a characteristic timescale of approximately 3 s, whereas the average lattice responds more slowly to heating. Upon removal of the heat source, the Bragg lattice recovers within approximately 11 s, while the superlattice re-establishes on nearly twice that timescale. These results reveal an asymmetric evolution of short- and long-range order under extreme non-equilibrium conditions, in which local PLD correlations are destroyed prior to, and recover more slowly than, the average lattice structure.
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Submitted 25 June, 2026; v1 submitted 18 September, 2025;
originally announced September 2025.
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Magnetic dynamics in NiTiO3 honeycomb antiferromagnet using neutron scattering
Authors:
Srimal Rathnayaka,
Luke Daemen,
Tao Hong,
Songxue Chi,
Stuart Calder,
John A. Schneeloch,
Yongqiang Cheng,
Bing Li,
Despina Louca
Abstract:
The ilmenite NiTiO3 consists of a buckled honeycomb lattice, with the Ni spins aligned ferromagnetically in-plane and antiferromagnetically out-of-plane. Using neutron spectroscopy, the magnetic structure and the dynamics were investigated as a function of temperature. Dispersive acoustic bands and nearly dispersionless optical bands at ~3.7 meV are described by a highly anisotropy Heisenberg mode…
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The ilmenite NiTiO3 consists of a buckled honeycomb lattice, with the Ni spins aligned ferromagnetically in-plane and antiferromagnetically out-of-plane. Using neutron spectroscopy, the magnetic structure and the dynamics were investigated as a function of temperature. Dispersive acoustic bands and nearly dispersionless optical bands at ~3.7 meV are described by a highly anisotropy Heisenberg model with stronger antiferromagnetic (AFM) out-of-plane, weaker ferromagnetic (FM) in-plane interactions and an anisotropy gap of 0.95 meV. The order parameter yields a critical exponent between the Heisenberg and two-dimensional Ising models, consistent with highly anisotropic Heisenberg systems. The frustration parameter ~ 2 supports a weakly frustrated system.
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Submitted 30 August, 2025;
originally announced September 2025.
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Helimagnetism in CrBr$_2$ and CrIBr
Authors:
John A. Schneeloch,
Adam A. Aczel,
Despina Louca
Abstract:
In CrX$_2$ (X=Br, I), a Jahn-Teller effect distorts the octahedral configuration of the anions about Cr, resulting in a "ribbon chain" structure. We previously observed helimagnetism in CrI$_2$ propagating along the ribbon chains, with an 80-90$^{\circ}$ rotation per Cr ion. Via neutron scattering, we report that CrBr$_2$ and the solid solution CrIBr are also helimagnetic, with Néel temperatures o…
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In CrX$_2$ (X=Br, I), a Jahn-Teller effect distorts the octahedral configuration of the anions about Cr, resulting in a "ribbon chain" structure. We previously observed helimagnetism in CrI$_2$ propagating along the ribbon chains, with an 80-90$^{\circ}$ rotation per Cr ion. Via neutron scattering, we report that CrBr$_2$ and the solid solution CrIBr are also helimagnetic, with Néel temperatures of 17 and 12 K, respectively, and signs of intermediate magnetic transitions in both compounds. The helical angle between spins on consecutive Cr ions along the ribbon chains increases with increasing Br substitution, from 89.7$^{\circ}$ (CrI$_2$) to 116$^{\circ}$ (CrIBr) to 147$^{\circ}$ (CrBr$_2$), possibly as a result of decreasing longer-range intrachain spin interactions with the increased electron localization of the lighter anions.
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Submitted 4 June, 2024;
originally announced June 2024.
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Role of stacking defects on the magnetic behavior of CrCl$_3$
Authors:
John A. Schneeloch,
Adam A. Aczel,
Feng Ye,
Despina Louca
Abstract:
In the study of van der Waals-layered magnetic materials, the properties of CrCl$_3$ continue to attract attention. This compound is reported to undergo antiferromagnetic (AFM) ordering below $\sim$14 K, with a ferromagneticlike region proposed to exist between 14 and 17 K. Ideally, the crystal structure is rhombohedral (R) below $\sim$235 K, separated from a higher-temperature monoclinic (M) phas…
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In the study of van der Waals-layered magnetic materials, the properties of CrCl$_3$ continue to attract attention. This compound is reported to undergo antiferromagnetic (AFM) ordering below $\sim$14 K, with a ferromagneticlike region proposed to exist between 14 and 17 K. Ideally, the crystal structure is rhombohedral (R) below $\sim$235 K, separated from a higher-temperature monoclinic (M) phase by a layer-sliding structural phase transition. However, the structural transition is often inhibited even in bulk single crystals, allowing M-type layer stacking, reported to have a tenfold greater interlayer magnetic coupling than R-type stacking, to be present at low temperature. To clarify the effect of stacking defects on CrCl$_3$, we report magnetization measurements on samples of varying crystalline quality. At low applied magnetic field, some crystals predominantly show the $T_N=14$ K peak, but other crystals show hysteretic behavior and a magnetization enhancement at a slightly higher temperature ($14 < T \lesssim 17$ K.) Samples with anomalous behavior exhibit a transition around $\sim$2 T in isothermal magnetization-field data, providing evidence that M-type stacking defects are the source of these anomalies. Ground powder samples are especially likely to show strongly anomalous behavior. We suggest that the anomalous behavior arises from few-layer magnetic domains that form just above $T_N$ in an environment of mixed interlayer magnetic coupling strength. We argue that the influence of M-type stacking boundaries on sublattice magnetization is already observable in reported neutron scattering data, and may be responsible for a certain feature in reported specific heat data.
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Submitted 21 May, 2024;
originally announced May 2024.
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Layer buckling and absence of superconductivity in LaNiO2
Authors:
S. Rathnayaka,
S. Yano,
K. Kawashima,
J. Akimitsu,
C. M. Brown,
J. Neuefeind,
D. Louca
Abstract:
The recent observation of unconventional superconductivity in thin films of LaNiO2 (critical temperature, Tc~10 K) and in bulk single crystals of La3Ni2O7 (327) under pressure (Tc~80 K), has brought to light a long sought-after class of superconducting nickelates. Through structural measurements in the 327-system, it was shown that the absence of superconductivity is related to bending of the O-Ni…
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The recent observation of unconventional superconductivity in thin films of LaNiO2 (critical temperature, Tc~10 K) and in bulk single crystals of La3Ni2O7 (327) under pressure (Tc~80 K), has brought to light a long sought-after class of superconducting nickelates. Through structural measurements in the 327-system, it was shown that the absence of superconductivity is related to bending of the O-Ni-O bonds. Similarly, the bond bending may be linked to the absence of superconductivity in bulk LaNiO2. Neutron diffraction was used on bulk non-superconducting La(1-x)Sr(x)NiO(2) samples to show that the layers are naturally buckled, creating a Ni-O-Ni bond angle of 177 at 2 K and ambient pressure. The buckling angle increases to 170 on warming to room temperature. Furthermore, a broad paramagnetic continuum is observed that decreases in intensity on cooling from room temperature signaling a possible transition to a coherent state. However, no antiferromagnetic (AFM) peaks are detected, although enhancement of ferromagnetic (FM) correlations cannot be excluded.
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Submitted 14 March, 2024;
originally announced March 2024.
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Observation of helimagnetism in the candidate ferroelectric CrI$_2$
Authors:
John A. Schneeloch,
Shunshun Liu,
Prasanna V. Balachandran,
Qiang Zhang,
Despina Louca
Abstract:
CrI$_{2}$ is a quasi-one dimensional (1D) van der Waals (vdW) system that exhibits helimagnetism that propagates along the ribbons. This was determined from neutron time-of-flight diffraction measurements. Below $T_N=17$ K, a screw-like helimagnetic order develops with an incommensurate wavevector of $\mathbf{q} \approx (0.2492,0,0)$ at 8 K. Using density functional theory (DFT)$+U$ calculations,…
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CrI$_{2}$ is a quasi-one dimensional (1D) van der Waals (vdW) system that exhibits helimagnetism that propagates along the ribbons. This was determined from neutron time-of-flight diffraction measurements. Below $T_N=17$ K, a screw-like helimagnetic order develops with an incommensurate wavevector of $\mathbf{q} \approx (0.2492,0,0)$ at 8 K. Using density functional theory (DFT)$+U$ calculations, the $J_{1}$-$J_{2}$ model was leveraged to describe the helimagnetism, where $J_{1} (> 0)$ and $J_2 (< 0)$ correspond, respectively, to a ferromagnetic nearest neighbor (NN) and antiferromagnetic next-nearest neighbor (NNN) intrachain interaction. The DFT$+U$ calculations predict that bulk CrI$_2$ in the orthorhombic $Cmc2_1$ crystal structure satisfies the $|J_2| > |J_1|/4$ condition, which favors formation of helimagnetic order.
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Submitted 18 October, 2023;
originally announced October 2023.
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Suppression of stacking order with doping in 1T-TaS$_{2-x}$Se$_x$
Authors:
Sharon S. Philip,
Despina Louca,
J. C. Neuefeind,
Matthew B. Stone,
A. I. Kolesnikov
Abstract:
In 1T-TaS$_{2-x}$Se$_x$, the charge density wave (CDW) state features a star of David lattice that expands across layers as the system becomes commensurate on cooling. The layers can also order along the c-axis and different stacking orders have been proposed. Using neutron scattering on powder samples, we compared the stacking order previously observed in 1T-TaS$_2$ as the system is doped with Se…
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In 1T-TaS$_{2-x}$Se$_x$, the charge density wave (CDW) state features a star of David lattice that expands across layers as the system becomes commensurate on cooling. The layers can also order along the c-axis and different stacking orders have been proposed. Using neutron scattering on powder samples, we compared the stacking order previously observed in 1T-TaS$_2$ as the system is doped with Se. While at low temperature, a 13c layer sequence stacking was observed in TaS$_2$, this type of ordering was not evident with doping. Doping with Se results in a nearly commensurate state with the Mott state suppressed which may be linked to the absence of the layer stacking.
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Submitted 23 September, 2023;
originally announced September 2023.
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Antiferromagnetic-ferromagnetic homostructures with Dirac magnons in van der Waals magnet CrI$_3$
Authors:
John A. Schneeloch,
Luke Daemen,
Despina Louca
Abstract:
Van der Waals (vdW) Dirac magnon system CrI$_3$, a potential host of topological edge magnons, orders ferromagnetically (FM) (T$_C=61$ K) in the bulk, but antiferromagnetic (AFM) order has been observed in nanometer thick flakes, attributed to monoclinic (M) type stacking. We report neutron scattering measurements on a powder sample where the usual transition to the rhombohedral (R) phase was inhi…
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Van der Waals (vdW) Dirac magnon system CrI$_3$, a potential host of topological edge magnons, orders ferromagnetically (FM) (T$_C=61$ K) in the bulk, but antiferromagnetic (AFM) order has been observed in nanometer thick flakes, attributed to monoclinic (M) type stacking. We report neutron scattering measurements on a powder sample where the usual transition to the rhombohedral (R) phase was inhibited for a majority of the structure. Elastic measurements (and the opening of a hysteresis in magnetization data on a pressed pellet) showed that an AFM transition is clearly present below $\sim$50 K, coexisting with the R-type FM order. Inelastic measurements showed a decrease in magnon energy compared to the R phase, consistent with a smaller interlayer magnetic coupling in M-type stacking. A gap remains at the Dirac point, suggesting that the same nontrivial magnon topology reported for the R phase may be present in the M phase as well.
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Submitted 19 May, 2023;
originally announced May 2023.
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Investigating the magneto-elastic properties in FeSn and Fe$_{3}$Sn$_{2}$ flat band metals
Authors:
Yu Tao,
Luke Daemen,
Yongqiang Cheng,
Joerg C. Neuefeind,
Despina Louca
Abstract:
Topological quantum magnets FeSn and Fe$_{3}$Sn$_{2}$ were studied using neutron scattering and first-principles calculations. Both materials are metallic but host dispersionless flat bands with Dirac nodes at the $K$ point in reciprocal space. The local structure determined from the pair density function analysis of the neutron diffraction data provided no evidence for electron localization in bo…
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Topological quantum magnets FeSn and Fe$_{3}$Sn$_{2}$ were studied using neutron scattering and first-principles calculations. Both materials are metallic but host dispersionless flat bands with Dirac nodes at the $K$ point in reciprocal space. The local structure determined from the pair density function analysis of the neutron diffraction data provided no evidence for electron localization in both compounds, consistent with their metallic nature. At the same time, in FeSn, an anomalous suppression in the $c$-axis lattice constant coupled with changes in the phonon spectra were observed across T$_{N}$ indicating the presence of magneto-elastic coupling and spin-phonon interactions. In addition, it was observed that spin waves persisted well above T$_{N}$, suggesting that the in-plane ferromagnetic spin correlations survive at high temperatures. In contrast, no lattice anomaly was observed in Fe$_{3}$Sn$_{2}$. The inelastic signal could be mostly accounted for by phonons, determined from density functional theory, showing typical softening on warming.
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Submitted 17 January, 2023;
originally announced January 2023.
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SEEMS: A Single Event Effects and Muon Spectroscopy facility at the Spallation Neutron Source
Authors:
Travis J. Williams,
Gregory J. MacDougall,
Bernie W. Riemer,
Franz X. Gallmeier,
Clarina R. dela Cruz,
Despina Louca
Abstract:
This manuscript outlines a concept that would leverage the existing proton accelerator at the Spallation Neutron Source of Oak Ridge National Laboratory to enable transformative science via one world-class facility serving two missions: Single Event Effects (SEE) and Muon Spectroscopy ($μ$SR). The $μ$SR portion would deliver the world's highest flux and highest resolution pulsed muon beams for mat…
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This manuscript outlines a concept that would leverage the existing proton accelerator at the Spallation Neutron Source of Oak Ridge National Laboratory to enable transformative science via one world-class facility serving two missions: Single Event Effects (SEE) and Muon Spectroscopy ($μ$SR). The $μ$SR portion would deliver the world's highest flux and highest resolution pulsed muon beams for materials characterization purposes, with precision and capabilities well beyond comparable facilities. The SEE capabilities deliver neutron, proton and muon beams for aerospace industries that are facing an impending challenge to certify equipment for safe and reliable behavior under bombardment from atmospheric radiation originating from cosmic and solar rays. With negligible impact on the primary neutron scattering mission of the SNS, the proposed facility will have enormous benefit for science and industry alike. We have designated this facility 'SEEMS'.
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Submitted 16 March, 2023; v1 submitted 19 December, 2022;
originally announced December 2022.
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A structural hysteresis in the charge density wave transition of 1T-TaS2
Authors:
Sharon S. Philip,
Despina Louca
Abstract:
In quasi-two-dimensional 1T-TaS2, a charge density wave (CDW) prototype, the transition occurs in two steps, from incommensurate (ICDW) and nearly commensurate (NCCDW) and from NCDW to commensurate (CCDW), locked in the resistivity step-wise behavior. The hysteresis observed in the resistivity across the NCDW-to-CCDW transition has roots to a structural hysteresis, where local distortions of the s…
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In quasi-two-dimensional 1T-TaS2, a charge density wave (CDW) prototype, the transition occurs in two steps, from incommensurate (ICDW) and nearly commensurate (NCCDW) and from NCDW to commensurate (CCDW), locked in the resistivity step-wise behavior. The hysteresis observed in the resistivity across the NCDW-to-CCDW transition has roots to a structural hysteresis, where local distortions of the sqrt(13)a x sqrt(13)a superstructure are revealed by neutron and X-ray diffraction. The structural hysteresis is due to faulty stars of David (SODs) because of Ta displacements away from the perfect trigonal geometry as well as out of plane S distortions. Furthermore, the superstructure exhibits a 3co layer stacking order that weakens on warming and fully disappears in the ICDW state.
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Submitted 13 November, 2022;
originally announced November 2022.
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Emergence of Layer Stacking Disorder in c-axis Confined MoTe$_2$
Authors:
James L Hart,
Lopa Bhatt,
Yanbing Zhu,
Myung-Geun Han,
Elisabeth Bianco,
Shunran Li,
David J Hynek,
John A Schneeloch,
Yu Tao,
Despina Louca,
Peijun Guo,
Yimei Zhu,
Felipe Jornada,
Evan J Reed,
Lena F Kourkoutis,
Judy J Cha
Abstract:
The layer stacking order in 2D materials strongly affects functional properties and holds promise for next generation electronic devices. In bulk, octahedral MoTe$_2$ possesses two stacking arrangements, the Weyl semimetal T$_d$ phase, and the higher-order topological insulator 1T' phase; however, it remains unclear if thin exfoliated flakes of MoTe$_2$ follow the T$_d$, 1T', or an alternative sta…
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The layer stacking order in 2D materials strongly affects functional properties and holds promise for next generation electronic devices. In bulk, octahedral MoTe$_2$ possesses two stacking arrangements, the Weyl semimetal T$_d$ phase, and the higher-order topological insulator 1T' phase; however, it remains unclear if thin exfoliated flakes of MoTe$_2$ follow the T$_d$, 1T', or an alternative stacking sequence. Here, we resolve this debate using atomic-resolution imaging within the transmission electron microscope. We find that the layer stacking in thin flakes of MoTe$_2$ is highly disordered and pseudo-random, which we attribute to intrinsic confinement effects. Conversely, WTe$_2$, which is isostructural and isoelectronic to MoTe$_2$, displays ordered stacking even for thin exfoliated flakes. Our results are important for understanding the quantum properties of MoTe$_2$ devices, and suggest that thickness may be used to alter the layer stacking in other 2D materials.
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Submitted 28 October, 2022;
originally announced October 2022.
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Lattice and magnetic dynamics in YVO$_{3}$ Mott insulator studied by neutron scattering and first-principles calculations
Authors:
Yu Tao,
Douglas L. Abernathy,
Tianran Chen,
Taner Yildirim,
Jiaqiang Yan,
Jianshi Zhou,
John B. Goodenough,
Despina Louca
Abstract:
The Mott insulator YVO$_{3}$ with $T_{N}$ = 118 K is revisited to explore the role of spin, lattice and orbital correlations across the multiple structural and magnetic transitions observed as a function of temperature. Upon cooling, the crystal structure changes from orthorhombic to monoclinic at 200 K, and back to orthorhombic at 77 K, followed by magnetic transitions. From the paramagnetic high…
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The Mott insulator YVO$_{3}$ with $T_{N}$ = 118 K is revisited to explore the role of spin, lattice and orbital correlations across the multiple structural and magnetic transitions observed as a function of temperature. Upon cooling, the crystal structure changes from orthorhombic to monoclinic at 200 K, and back to orthorhombic at 77 K, followed by magnetic transitions. From the paramagnetic high temperature phase, C-type ordering is first observed at 118 K, followed by a G-type spin re-orientation transition at 77 K. The dynamics of the transitions were investigated via inelastic neutron scattering and first principles calculations. An overall good agreement between the neutron data and calculated spectra was observed. From the magnon density of states, the magnetic exchange constants were deduced to be $J_{ab}$ = $J_{c}$ = -5.8 meV in the G-type spin phase, and $J_{ab}$ = -3.8 meV, $J_{c}$ = 7.6 meV at 80 K and $J_{ab}$ = -3.0 meV, $J_{c}$ = 6.0 meV at 100 K in the C-type spin phase. Paramagnetic scattering was observed in the spin ordered phases, well below the C-type transition temperature, that continuously increased above the transition. Fluctuations in the temperature dependence of the phonon density of states were observed between 50 and 80 K as well, coinciding with the G-type to C-type transition. These fluctuations are attributed to optical oxygen modes above 40 meV, from first principles calculations. In contrast, little change in the phonon spectra is observed across $T_{N}$.
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Submitted 24 December, 2021;
originally announced December 2021.
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Charge-ordered state satisfying the Anderson condition in LiRh2O4 arising from local dimer order
Authors:
Manabu Shiomi,
Keita Kojima,
Naoyuki Katayama,
Shin Maeda,
John A. Schneeloch,
Syunsuke Yamamoto,
Koudai Sugimoto,
Yukinori Ohta,
Despina Louca,
Yoshihiko Okamoto,
Hiroshi Sawa
Abstract:
We report on the charge-ordered structure of LiRh2O4 arising below the metal-insulator transition at 170 K. Structural studies using synchrotron X-rays have revealed that the charge-ordered states of Rh3+ and Rh4+ with dimerization are realized in the low-temperature phase below 170 K. Although the low-temperature ground state resembles that of CuIr2S4, a charge ordering pattern satisfying the And…
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We report on the charge-ordered structure of LiRh2O4 arising below the metal-insulator transition at 170 K. Structural studies using synchrotron X-rays have revealed that the charge-ordered states of Rh3+ and Rh4+ with dimerization are realized in the low-temperature phase below 170 K. Although the low-temperature ground state resembles that of CuIr2S4, a charge ordering pattern satisfying the Anderson condition is realized in LiRh2O4. Based on structural information such as the short-range order of dimers appearing above the transition temperature and the weakening of the correlation between rhodium one-dimensional chains appearing in the crystal structure, we argue that the Coulomb interaction plays an important role in determining the charge ordering patterns.
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Submitted 14 December, 2021; v1 submitted 13 December, 2021;
originally announced December 2021.
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Large change of interlayer vibrational coupling with stacking in Mo$_{1-x}$W$_{x}$Te$_{2}$
Authors:
John A. Schneeloch,
Yu Tao,
Jaime A. Fernandez-Baca,
Guangyong Xu,
Despina Louca
Abstract:
Stacking variations in quasi-2D materials can have an important influence on material properties, such as changing the topology of the band structure. Unfortunately, the weakness of van der Waals interactions makes it difficult to compute the stacking dependence of properties, and even in a material as simple as graphite the stacking energetics remain unclear. Mo$_{1-x}$W$_{x}$Te$_{2}$ is a materi…
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Stacking variations in quasi-2D materials can have an important influence on material properties, such as changing the topology of the band structure. Unfortunately, the weakness of van der Waals interactions makes it difficult to compute the stacking dependence of properties, and even in a material as simple as graphite the stacking energetics remain unclear. Mo$_{1-x}$W$_{x}$Te$_{2}$ is a material in which three differently-stacked phases are conveniently accessible by temperature changes: $1T^{\prime}$, $T^*_d$, and the reported Weyl semimetal phase $T_d$. The transitions proceed via layer sliding, and the corresponding interlayer shear mode (ISM) is relevant not just for the stacking energetics, but for understanding the relationship between the Weyl physics and structural changes. However, the interlayer interactions of Mo$_{1-x}$W$_{x}$Te$_{2}$ are not well understood, with wide variation in computed properties. We report inelastic neutron scattering of the ISM in a Mo$_{0.91}$W$_{0.09}$Te$_{2}$ crystal. The ISM energies are generally consistent with the linear chain model (LCM), as expected given the weak interlayer interaction, though there are some discrepancies from predicted intensities. However, the interlayer force constants $K_x$ in the $T^*_d$ and $1T^{\prime}$ phases are substantially weaker than that of $T_d$, at 76(3)% and 83(3)%, respectively. Considering that the relative positioning of atoms in neighboring layers is approximately the same regardless of overall stacking, our results suggest that longer-range influences, such as stacking-induced band structure changes, may be responsible for the substantial change in the interlayer vibrational coupling. These findings should elucidate the stacking energetics of Mo$_{1-x}$W$_{x}$Te$_{2}$ and other van der Waals layered materials.
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Submitted 20 October, 2021;
originally announced October 2021.
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Gapless Dirac magnons in CrCl$_{3}$
Authors:
John A. Schneeloch,
Yu Tao,
Yongqiang Cheng,
Luke Daemen,
Guangyong Xu,
Qiang Zhang,
Despina Louca
Abstract:
Bosonic Dirac materials are testbeds for dissipationless spin-based electronics. In the quasi two-dimensional honeycomb lattice of CrX$_{3}$ (X=Cl, Br, I), Dirac magnons have been predicted at the crossing of acoustical and optical spin waves, analogous to Dirac fermions in graphene. Here we show that, distinct from CrBr$_{3}$ and CrI$_{3}$, gapless Dirac magnons are present in bulk CrCl$_{3}$, wi…
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Bosonic Dirac materials are testbeds for dissipationless spin-based electronics. In the quasi two-dimensional honeycomb lattice of CrX$_{3}$ (X=Cl, Br, I), Dirac magnons have been predicted at the crossing of acoustical and optical spin waves, analogous to Dirac fermions in graphene. Here we show that, distinct from CrBr$_{3}$ and CrI$_{3}$, gapless Dirac magnons are present in bulk CrCl$_{3}$, with inelastic neutron scattering intensity at low temperatures approaching zero at the Dirac $K$ point. Upon warming, magnon-magnon interactions induce strong renormalization and decreased lifetimes, with a ~25% softening of the upper magnon branch intensity from 5 to 50 K, though magnon features persist well above T$_{N}$. Moreover, an unusual negative thermal expansion (NTE) of the $a$-axis lattice constant and anomalous phonon behavior are observed below 50 K, indicating magnetoelastic and spin-phonon coupling arising from an increase in the in-plane spin correlations that begins tens of Kelvin above T$_{N}$.
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Submitted 20 October, 2021;
originally announced October 2021.
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Bi kagome sublattice distortions by quenching and flux pinning in superconducting RbBi$_2$
Authors:
Sharon S. Philip,
Junjie Yang,
P. F. S. Rosa,
J. D. Thompson,
K. L. Page,
Despina Louca
Abstract:
The properties of RbBi$_2$, a 4.15 K superconductor, were investigated using magnetic field, pressure and neutron diffraction. Under hydrostatic pressure, an almost 50 % reduction of T$_c$ is observed, linked to a low Debye temperature estimated at 165 K. The resistivity and magnetic susceptibility were measured on quenched and slow-cooled polycrystalline samples. The resistivity follows a low tem…
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The properties of RbBi$_2$, a 4.15 K superconductor, were investigated using magnetic field, pressure and neutron diffraction. Under hydrostatic pressure, an almost 50 % reduction of T$_c$ is observed, linked to a low Debye temperature estimated at 165 K. The resistivity and magnetic susceptibility were measured on quenched and slow-cooled polycrystalline samples. The resistivity follows a low temperature power-law dependence in both types of samples, while the diamagnetic susceptibility, $χ$, is dependent on the sample cooling history. Slow-cooled samples have a $χ= -1$ while quenched samples have $χ< -1$ due to grain size differences. Evidence of the effects of the cooling rate is also discerned from the local structure, obtained by neutron diffraction and the pair density function analysis. Slow-cooled samples have structurally symmetric Bi hexagons, in contrast to quenched samples in which disorder is manifested in periodic distortions of the Bi hexagonal rings of the kagome sublattice. Disorder may lead to flux pinning that reduces vortex mobility, but T$_c$ remains unaffected by the cooling rate.
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Submitted 11 October, 2021;
originally announced October 2021.
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T$_{d}$ to 1T$^{\prime}$ structural phase transition in WTe$_{2}$ Weyl semimetal
Authors:
Yu Tao,
John A. Schneeloch,
Adam A. Aczel,
Despina Louca
Abstract:
Elastic neutron scattering on a single crystal and powder X-ray diffraction measurements were carried out to investigate how the crystal structure evolves as a function of temperature in the Weyl semimetal WTe$_{2}$. A sharp transition from the low-temperature orthorhombic phase (T$_{d}$) to the high-temperature monoclinic phase (1T$^{\prime}$) was observed at ambient pressure in the single crysta…
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Elastic neutron scattering on a single crystal and powder X-ray diffraction measurements were carried out to investigate how the crystal structure evolves as a function of temperature in the Weyl semimetal WTe$_{2}$. A sharp transition from the low-temperature orthorhombic phase (T$_{d}$) to the high-temperature monoclinic phase (1T$^{\prime}$) was observed at ambient pressure in the single crystal near $\sim$565 K. Unlike in MoTe$_{2}$, the solid-solid transition from T$_{d}$ to 1T$^{\prime}$ occurs without the cell doubling of the intermediate T$_{d}^{*}$ phase with AABB (or ABBA) layer stacking. In powders however, the thermal transition from the T$_{d}$ to the 1T$^{\prime}$ phase is broadened and a two phase coexistence was observed until 700K, well above the structural transition.
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Submitted 22 June, 2020; v1 submitted 20 March, 2020;
originally announced March 2020.
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Evolution of the structural transition in Mo$_{1-x}$W$_{x}$Te$_{2}$
Authors:
John A. Schneeloch,
Yu Tao,
Chunruo Duan,
Masaaki Matsuda,
Adam A. Aczel,
Jaime A. Fernandez-Baca,
Guangyong Xu,
Jörg C. Neuefeind,
Junjie Yang,
Despina Louca
Abstract:
The composition dependence of the structural transition between the monoclinic 1T$^{\prime}$ and orthorhombic T$_{d}$ phases in the Mo$_{1-x}$W$_{x}$Te$_{2}$ Weyl semimetal was investigated by elastic neutron scattering on single crystals up to $x \approx 0.54$. First observed in MoTe$_{2}$, the transition from T$_{d}$ to 1T$^{\prime}$ is accompanied by an intermediate pseudo-orthorhombic phase, T…
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The composition dependence of the structural transition between the monoclinic 1T$^{\prime}$ and orthorhombic T$_{d}$ phases in the Mo$_{1-x}$W$_{x}$Te$_{2}$ Weyl semimetal was investigated by elastic neutron scattering on single crystals up to $x \approx 0.54$. First observed in MoTe$_{2}$, the transition from T$_{d}$ to 1T$^{\prime}$ is accompanied by an intermediate pseudo-orthorhombic phase, T$_{d}^{*}$. Upon doping with W, the T$_{d}^{*}$ phase vanishes by $x \approx 0.34$. Above this concentration, a phase coexistence behavior with both T$_{d}$ and 1T$^{\prime}$ is observed instead. The interlayer in-plane positioning parameter $δ$, which relates to the 1T$^{\prime}$ $β$ 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 $x \approx 0.54$, in contrast to the broadening reported under pressure.
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Submitted 11 June, 2020; v1 submitted 18 March, 2020;
originally announced March 2020.
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Charge Density Modulation and Defect Ordering in Na$_x$MnBi$_y$ magnetic semimetal
Authors:
Aaron Wegner,
Despina Louca,
Keith Taddei,
Joerg Neuefeind
Abstract:
The I-Mn-V antiferromagnet, NaMnBi, develops a very large positive magnetoresistance (MR) up to 10,000% at 2 K and 9 T in crystals showing a semiconductor-to-metal transition (SMT). In the absence of an SMT, a modest (20%) MR is achieved. Here, we show that upon cooling below the magnetic transition, a spatial modulation appears giving rise to new Bragg peaks due to charge and defect ordering in a…
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The I-Mn-V antiferromagnet, NaMnBi, develops a very large positive magnetoresistance (MR) up to 10,000% at 2 K and 9 T in crystals showing a semiconductor-to-metal transition (SMT). In the absence of an SMT, a modest (20%) MR is achieved. Here, we show that upon cooling below the magnetic transition, a spatial modulation appears giving rise to new Bragg peaks due to charge and defect ordering in a checkerboard pattern, with two kinds of modulation vectors, $q_1$=($\frac23$, 0, 1) and $q_2$=($\frac23, \frac13, \frac12$). This constitutes a superlattice transition ($T_s$) that lowers the symmetry from the high temperature centrosymmetric P4/nmm to the non-centrosymmetric P$\overline4$m2. In crystals with a large MR, a close to room temperature $T_s$ is observed with $q_1$ appearing first, followed by $q_2$. In crystals with low MR however, $T_s$ is much lower and only $q_1$ is observed. The charge modulation and spin fluctuations may both contribute to the enhancement of MR.
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Submitted 28 February, 2020;
originally announced March 2020.
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Appearance of T$_d^*$ phase across the T$_{d}$-1T$^{\prime}$ phase boundary in Weyl semimetal MoTe$_{2}$
Authors:
Yu Tao,
John A. Schneeloch,
Chunruo Duan,
Masaaki Matsuda,
Sachith E. Dissanayake,
Adam A. Aczel,
Jaime A. Fernandez-Baca,
Feng Ye,
Despina Louca
Abstract:
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…
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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.
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Submitted 26 August, 2019; v1 submitted 18 February, 2019;
originally announced February 2019.
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Emergence of topologically protected states in MoTe$_{2}$ Weyl semimetal with layer stacking order
Authors:
John A. Schneeloch,
Chunruo Duan,
Xiaoping Wang,
Jun Liu,
Junjie Yang,
Despina Louca
Abstract:
Electronic tunability in crystals with weakly-bound layers can be achieved through layer stacking order. One such example is MoTe$_2$, where the low-temperature orthorhombic T$_d$ phase is topological and host to Weyl quasiparticles. The transition mechanism to the non-trivial topology is elucidated by single crystal neutron diffraction. Upon cooling from the monoclinic 1T$\prime$ to the T$_d$ pha…
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Electronic tunability in crystals with weakly-bound layers can be achieved through layer stacking order. One such example is MoTe$_2$, where the low-temperature orthorhombic T$_d$ phase is topological and host to Weyl quasiparticles. The transition mechanism to the non-trivial topology is elucidated by single crystal neutron diffraction. Upon cooling from the monoclinic 1T$\prime$ to the T$_d$ phase, diffuse scattering accompanies the transition, arising from random, in-plane layer displacements, and dissipates upon entering the T$_d$ phase. Diffuse scattering is observed only in the H0L plane due to irreversible layer shifts along the c-axis that break the centrosymmetry of the monoclinic lattice.
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Submitted 15 February, 2019; v1 submitted 17 August, 2018;
originally announced August 2018.
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Evidence for breathing-type pseudo Jahn-Teller distortions in the charge density wave phase of 1$T$-TiSe$_2$
Authors:
A. Wegner,
J. Zhao,
J. Li,
J. Yang,
A. A. Anikin,
G. Karapetrov,
D. Louca,
U. Chatterjee
Abstract:
The charge density wave (CDW) phase in 1$T$-TiSe$_2$ is investigated using angle resolved photoemission spectroscopy (ARPES) and neutron scattering measurements. Our ARPES results reveal a clear temperature dependence of the chemical potential of the system. They also demonstrate specific changes encountered by the Se 4$p$ valence and Ti 3$d$ conduction bands as the temperature of the system is de…
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The charge density wave (CDW) phase in 1$T$-TiSe$_2$ is investigated using angle resolved photoemission spectroscopy (ARPES) and neutron scattering measurements. Our ARPES results reveal a clear temperature dependence of the chemical potential of the system. They also demonstrate specific changes encountered by the Se 4$p$ valence and Ti 3$d$ conduction bands as the temperature of the system is decreased through $T_{\text{CDW}}$. The valence band undergoes a downward shift, whereas the conduction band remains unaffected. The crystal structure in the CDW state shows a distinct split of the Ti-Se atomic correlations that are reminiscent of Jahn-Teller distortions, manifested in a breathing-type mode. The ARPES data together with the local structure analysis support a direct link between Jahn-Teller-like distortions and the CDW order in 1$T$-TiSe$_2$.
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Submitted 15 July, 2018;
originally announced July 2018.
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Orbital selectivity causing anisotropy and particle-hole asymmetry in the charge density wave gap of $2H$-TaS$_2$
Authors:
J. Zhao,
K. Wijayaratne,
A. Butler,
V. Karlapati,
J. Yang,
C. D. Malliakas,
D. Y. Chung,
D. Louca,
M. G. Kanatzidis,
J. van Wezel,
U. Chatterjee
Abstract:
We report an in-depth Angle Resolved Photoemission Spectroscopy (ARPES) study on $2H$-TaS$_2$, a canonical incommensurate Charge Density Wave (CDW) system. This study demonstrates that just as in related incommensurate CDW systems, $2H$-TaSe$_2$ and $2H$-NbSe$_2$, the energy gap ($Δ_{\text{cdw}}\,$) of $2H$-TaS$_2$ is localized along the K-centered Fermi surface barrels and is particle-hole asymme…
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We report an in-depth Angle Resolved Photoemission Spectroscopy (ARPES) study on $2H$-TaS$_2$, a canonical incommensurate Charge Density Wave (CDW) system. This study demonstrates that just as in related incommensurate CDW systems, $2H$-TaSe$_2$ and $2H$-NbSe$_2$, the energy gap ($Δ_{\text{cdw}}\,$) of $2H$-TaS$_2$ is localized along the K-centered Fermi surface barrels and is particle-hole asymmetric. The persistence of $Δ_{\text{cdw}}\,$ even at temperatures higher than the CDW transition temperature $\it{T}_{\text{cdw}}\,$ in $2H$-TaS$_2$, reflects the similar pseudogap (PG) behavior observed previously in $2H$-TaSe$_2$ and $2H$-NbSe$_2$. However, in sharp contrast to $2H$-NbSe$_2$, where $Δ_{\text{cdw}}\,$ is non-zero only in the vicinity of a few "hot spots" on the inner K-centered Fermi surface barrels, $Δ_{\text{cdw}}\,$ in $2H$-TaS$_2$ is non-zero along the entirety of both K-centered Fermi surface barrels. Based on a tight-binding model, we attribute this dichotomy in the momentum dependence and the Fermi surface specificity of $Δ_{\text{cdw}}\,$ between otherwise similar CDW compounds to the different orbital orientations of their electronic states that are involved in CDW pairing. Our results suggest that the orbital selectivity plays a critical role in the description of incommensurate CDW materials.
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Submitted 7 May, 2018;
originally announced May 2018.
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Elastic and electronic tuning of magnetoresistance in MoTe$_2$
Authors:
Junjie Yang,
Jonathan Colen,
Jun Liu,
Manh Cuong Nguyen,
Gia-Wei Chern,
Despina Louca
Abstract:
Quasi-two dimensional transition metal dichalcogenides (TMD) exhibit dramatic properties that may transform electronic and photonic devices. We report on how the anomalously large magnetoresistance (MR) observed under high magnetic field in MoTe$_2$, a type II Weyl semimetal, can be reversibly controlled under tensile strain. The MR is enhanced by as much as ~ 30 % at low temperatures and high mag…
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Quasi-two dimensional transition metal dichalcogenides (TMD) exhibit dramatic properties that may transform electronic and photonic devices. We report on how the anomalously large magnetoresistance (MR) observed under high magnetic field in MoTe$_2$, a type II Weyl semimetal, can be reversibly controlled under tensile strain. The MR is enhanced by as much as ~ 30 % at low temperatures and high magnetic fields, when uniaxial strain is applied along the $a$-crystallographic direction and reduced by about the same amount when strain is applied along the $b$-direction. We show that the large in-plane electric anisotropy is coupled with the structural transition from the 1T' monoclinic to the Td orthorhombic Weyl phase. A shift of the Td - 1T' phase boundary is achieved by minimal tensile strain. The sensitivity of the MR to tensile strain suggests the possibility of a nontrivial spin-orbital texture of the electron and hole pockets in the vicinity of Weyl points. Our ab initio calculations indeed show a significant orbital mixing on the Fermi surface, which is modified by the tensile strains.
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Submitted 6 October, 2017;
originally announced October 2017.
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Charge Fluctuations in the NdO$_{1-x}$F$_{x}$BiS$_{2}$ Superconductors
Authors:
Anushika Athauda,
Yoshikazu Mizuguchi,
Masanori Nagao,
Joerg Neuefeind,
Despina Louca
Abstract:
The local atomic structure of superconducting NdO$_{1-x}$F$_{x}$BiS$_{2}$ ($x$=0.2 and 0.4) is investigated using neutron diffraction and the pair density function analysis technique. In the non-superconducting $x$=0.2 composition, ferrodistortive displacements of the pyramidal sulfur ions break the tetragonal symmetry and a superlattice structure emerges with peaks appearing at $h+k$ odd reflecti…
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The local atomic structure of superconducting NdO$_{1-x}$F$_{x}$BiS$_{2}$ ($x$=0.2 and 0.4) is investigated using neutron diffraction and the pair density function analysis technique. In the non-superconducting $x$=0.2 composition, ferrodistortive displacements of the pyramidal sulfur ions break the tetragonal symmetry and a superlattice structure emerges with peaks appearing at $h+k$ odd reflections superimposed on the even reflections of the $P4/nmm$ symmetry. In the superconducting $x$=0.4 composition, similar ferrodistortive displacements are observed but with different magnitudes coupled with in-plane Bi distortions. The distortions are indicative of charge fluctuations that may lead to charge localization and suppression of superconductivity.
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Submitted 13 August, 2017;
originally announced August 2017.
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Superconductivity at the vacancy disorder boundary in K$_x$Fe$_{2-y}$Se$_2$
Authors:
Chunruo Duan,
Junjie Yang,
Yang Ren,
Despina Louca
Abstract:
The role of phase separation in the emergence of superconductivity in alkali metal doped iron selenides A$_{x}$Fe$_{2-y}$Se$_{2}$ (A = K, Rb, Cs) is revisited. High energy X-ray diffraction and Monte Carlo simulation were used to investigate the crystal structure of quenched superconducting (SC) and as-grown non-superconducting (NSC) K$_{x}$Fe$_{2-y}$Se$_{2}$ single crystals. The coexistence of su…
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The role of phase separation in the emergence of superconductivity in alkali metal doped iron selenides A$_{x}$Fe$_{2-y}$Se$_{2}$ (A = K, Rb, Cs) is revisited. High energy X-ray diffraction and Monte Carlo simulation were used to investigate the crystal structure of quenched superconducting (SC) and as-grown non-superconducting (NSC) K$_{x}$Fe$_{2-y}$Se$_{2}$ single crystals. The coexistence of superlattice structures with the in-plane $\sqrt{2}\times\sqrt{2}$ K-vacancy ordering and the $\sqrt{5}\times\sqrt{5}$ Fe-vacancy ordering were observed in SC and NSC crystals along side the \textit{I4/mmm} Fe-vacancy free phase. Moreover, in the SC crystal an Fe-vacancy disordered phase is additionally present. It appears at the boundary between the \textit{I4/mmm} vacancy free phase and the \textit{I4/m} vacancy ordered phase ($\sqrt{5}\times\sqrt{5}$). The vacancy disordered phase is most likely the host of superconductivity.
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Submitted 3 August, 2017; v1 submitted 7 June, 2017;
originally announced June 2017.
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Ferro-lattice-distortions and charge fluctuations in superconducting LaO$_{1-x}$F$_{x}$BiS$_{2}$
Authors:
A. Athauda,
C. Hoffman,
Y. Ren,
S. Aswartham,
J. Terzic,
G. Cao,
X. Zhu,
D. Louca
Abstract:
Competing ferroelectric and charge density wave phases have been proposed to be present in the electron-phonon coupled LaO$_{1-x}$F$_{x}$BiS$_{2}$ superconductor. The lattice instability arises from unstable phonon modes that can break the crystal symmetry. Upon examination of the crystal structure using single crystal diffraction, we find a superlattice pattern arising from coherent in-plane disp…
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Competing ferroelectric and charge density wave phases have been proposed to be present in the electron-phonon coupled LaO$_{1-x}$F$_{x}$BiS$_{2}$ superconductor. The lattice instability arises from unstable phonon modes that can break the crystal symmetry. Upon examination of the crystal structure using single crystal diffraction, we find a superlattice pattern arising from coherent in-plane displacements of the sulfur atoms in the BiS$_{2}$ superconducting planes. The distortions morph into coordinated ferro-distortive patterns, challenging previous symmetry suggestions including the possible presence of unstable antiferro-distortive patterns. The ferro-distortive pattern remains in the superconducting state, but with the displacements diminished in magnitude. Moreover, the sulfur displacements can exist in several polytypes stacked along the c-axis. Charge carriers can get trapped in the lattice deformations reducing the effective number of carriers available for pairing.
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Submitted 27 January, 2016;
originally announced January 2016.
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In-plane Charge Fluctuations in Bismuth Sulfide Superconductors
Authors:
Anushika Athauda,
Junjie Yang,
Seunghun Lee,
Yoshikazu Mizuguchi,
Keita Deguchi,
Yoshihiko Takano,
Osuke Miura,
Despina Louca
Abstract:
Evidence for local charge fluctuations linked to a charge disproportionation of the Bi ions in the distorted lattice of superconducting LaO$_{1-x}$F$_{x}$ BiS$_{2}$ is presented. In-plane short-range distortions of sulfur atoms up to 0.3 Å in magnitude break site symmetry and create two distinct environments around Bi. Out-of-plane motion of apical sulfur brings it closer to the La-O/F doping laye…
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Evidence for local charge fluctuations linked to a charge disproportionation of the Bi ions in the distorted lattice of superconducting LaO$_{1-x}$F$_{x}$ BiS$_{2}$ is presented. In-plane short-range distortions of sulfur atoms up to 0.3 Å in magnitude break site symmetry and create two distinct environments around Bi. Out-of-plane motion of apical sulfur brings it closer to the La-O/F doping layer with increasing $x$ that may lead to a charge transfer conduit between the doping layers and the superconducting BiS$_{2}$ planes. The mechanism for superconductivity may arise from the interplay between charge density fluctuations and an enhanced spin-orbit coupling suggested theoretically, that induces spin polarization.
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Submitted 8 March, 2015;
originally announced March 2015.
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Coexistence of ferromagnetism and superconductivity in CeO$_{0.3}$F$_{0.7}$BiS$_{2}$
Authors:
J. Lee,
S. Demura,
M. B. Stone,
K. Iida,
G. Ehlers,
C. R. dela Cruz,
M. Matsuda,
K. Deguchi,
Y. Takano,
Y. Mizuguchi,
O. Miura,
D. Louca,
S. -H. Lee
Abstract:
Bulk magnetization, transport and neutron scattering measurements were performed to investigate the electronic and magnetic properties of a polycrystalline sample of the newly discovered ferromagnetic superconductor, CeO$_{0.3}$F$_{0.7}$BiS$_{2}$. Ferromagnetism develops below T$_{FM}$ = 6.54(8) K and superconductivity is found to coexist with the ferromagnetic state below T$_{SC}$ ~ 4.5 K. Inelas…
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Bulk magnetization, transport and neutron scattering measurements were performed to investigate the electronic and magnetic properties of a polycrystalline sample of the newly discovered ferromagnetic superconductor, CeO$_{0.3}$F$_{0.7}$BiS$_{2}$. Ferromagnetism develops below T$_{FM}$ = 6.54(8) K and superconductivity is found to coexist with the ferromagnetic state below T$_{SC}$ ~ 4.5 K. Inelastic neutron scattering measurements reveal a very weakly dispersive magnetic excitation at 1.8 meV that can be explained by an Ising-like spin Hamiltonian. Under application of an external magnetic field, the direction of the magnetic moment changes from the c-axis to the ab-plane and the 1.8 meV excitation splits into two modes. A possible mechanism for the unusual magnetism and its relation to superconductivity is discussed.
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Submitted 12 November, 2014;
originally announced November 2014.
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Structure and composition of the superconducting phase in alkali iron selenide K$_y$Fe$_{1.6+x}$Se$_2$
Authors:
Scott V Carr,
Despina Louca,
Joan Siewenie,
Q. Huang,
Aifeng Wang,
Xianhui Chen,
Pengcheng Dai
Abstract:
We use neutron diffraction to study the temperature evolution of the average structure and local lattice distortions in insulating and superconducting potassium iron selenide K$_y$Fe$_{1.6+x}$Se$_2$. In the high temperature paramagnetic state, both materials have a single phase with crystal structure similar to that of the BaFe$_2$As$_2$ family of iron pnictides. While the insulating K$_y$Fe…
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We use neutron diffraction to study the temperature evolution of the average structure and local lattice distortions in insulating and superconducting potassium iron selenide K$_y$Fe$_{1.6+x}$Se$_2$. In the high temperature paramagnetic state, both materials have a single phase with crystal structure similar to that of the BaFe$_2$As$_2$ family of iron pnictides. While the insulating K$_y$Fe$_{1.6+x}$Se$_2$ forms a $\sqrt{5}\times\sqrt{5}$ iron vacancy ordered block antiferromagnetic (AF) structure at low-temperature, the superconducting compounds spontaneously phase separate into an insulating part with $\sqrt{5}\times\sqrt{5}$ iron vacancy order and a superconducting phase with chemical composition of K$_z$Fe$_{2}$Se$_2$ and BaFe$_2$As$_2$ structure. Therefore, superconductivity in alkaline iron selenides arises from alkali deficient K$_z$Fe$_{2}$Se$_2$ in the matrix of the insulating block AF phase.
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Submitted 14 April, 2014;
originally announced April 2014.
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The hybrid lattice of KxFe2-ySe2: why superconductivity and magnetism can coexist
Authors:
Despina Louca,
Keeseong Park,
Bing Li,
Joerg Neuefeind,
Jiaqiang Yan
Abstract:
Much remains unknown of the microscopic origin of superconductivity when it materializes in atomically disordered systems as in amorphous alloys (1) or in crystals riddled with defects(2). A manifestation of this conundrum is envisaged in the highly defective iron chalcogenide superconductors of KxFe2-ySe2 (3-6). How can superconductivity survive under such crude conditions that call for strong el…
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Much remains unknown of the microscopic origin of superconductivity when it materializes in atomically disordered systems as in amorphous alloys (1) or in crystals riddled with defects(2). A manifestation of this conundrum is envisaged in the highly defective iron chalcogenide superconductors of KxFe2-ySe2 (3-6). How can superconductivity survive under such crude conditions that call for strong electron localization (7)? With vacancies present both at the K and Fe sites, superconductivity is bordering a semi-metallic region below x ~ 0.7 and an insulating and antiferromagnetic region above x ~ 0.85 (8,9). Here, we report on the bulk local atomic structure and show that the Fe sublattice is locally distorted in a way that it accommodates two kinds of Fe valence environments giving rise to a bimodal bond distribution. While the bond length distribution is driven by K and Fe contents, the superconducting state is characterized by the coexistence of both short (metallic) and long (insulating) Fe bond environments and is not phase separated. In contrast to other Fe-based materials in which only one kind of Fe to Fe bond is present, the dual nature of the Fe correlations explains why superconductivity is intertwined with magnetic order. Such a hybrid state is most likely present in cuprate superconductors as well (10,11) while our results point to the importance of the local atomic symmetry by which the exchange interactions between local moments can materialize (12).
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Submitted 8 February, 2013;
originally announced February 2013.
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Possible link of a structurally driven spin flip transition and the insulator-metal transition in the perovskite La$_{1-x}$Ba$_{x}$CoO$_{3}$
Authors:
Peng Tong,
Juan Yu,
Qingzhen Huang,
Kazuyoshi Yamada,
Despina Louca
Abstract:
The complex nature of the magnetic ground state in La$_{1-x}$A$_{x}$CoO$_{3}$ (A = Ca, Sr, Ba) has been investigated via neutron scattering. It was previously observed that ferromagnetic (FM) as well as antiferromagnetic (AFM) correlations can coexist prior to the insulator-metal transition (IMT). We focused on a unique region in the Ba phase diagram, from x = 0.17 - 0.22, in which a commensurate…
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The complex nature of the magnetic ground state in La$_{1-x}$A$_{x}$CoO$_{3}$ (A = Ca, Sr, Ba) has been investigated via neutron scattering. It was previously observed that ferromagnetic (FM) as well as antiferromagnetic (AFM) correlations can coexist prior to the insulator-metal transition (IMT). We focused on a unique region in the Ba phase diagram, from x = 0.17 - 0.22, in which a commensurate AFM phase appears first with a propagation vector, k = (0, -0.5, 0.5), and the Co moment in the (001)$_{R}$ plane of the rhombohedral lattice. With increasing x, the AFM component weakens while an FM order appears with the FM Co moment directed along the (001)$_{R}$ (=(111)$_{C}$) axis. By x = 0.22, a spin flip to new FM component appears as the crystal fully transforms to an orthorhombic (Pnma) structure, with the Co moments pointing along a new direction, (001)$_{O}$ (=(110)$_{C}$). It is the emergence of the magnetic Pnma phase that leads to IMT.
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Submitted 25 March, 2010;
originally announced March 2010.
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Investigation of the spin-glass regime between the antiferromagnetic and superconducting phases in Fe$_{1+y}$Se$_x$Te$_{1-x}$
Authors:
N. Katayama,
S. Ji,
D. Louca,
S. -H. Lee,
M. Fujita,
T. J. Sato,
J. S. Wen,
Z. J. Xu,
G. D. Gu,
G. Xu,
Z. W. Lin,
M. Enoki,
S. Chang,
K. Yamada,
J. M. Tranquada
Abstract:
Using bulk magnetization along with elastic and inelastic neutron scattering techniques, we have investigated the phase diagram of Fe$_{1+y}$Se$_{x}$Te$_{1-x}$ and the nature of magnetic correlations in three nonsuperconducting samples of Fe$_{1.01}$Se$_{0.1}$Te$_{0.9}$, Fe$_{1.01}$Se$_{0.15}$Te$_{0.85}$ and Fe$_{1.02}$Se$_{0.3}$Te$_{0.7}$. A cusp and hysteresis in the temperature dependence of t…
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Using bulk magnetization along with elastic and inelastic neutron scattering techniques, we have investigated the phase diagram of Fe$_{1+y}$Se$_{x}$Te$_{1-x}$ and the nature of magnetic correlations in three nonsuperconducting samples of Fe$_{1.01}$Se$_{0.1}$Te$_{0.9}$, Fe$_{1.01}$Se$_{0.15}$Te$_{0.85}$ and Fe$_{1.02}$Se$_{0.3}$Te$_{0.7}$. A cusp and hysteresis in the temperature dependence of the magnetization for the $x=0.15$ and 0.3 samples indicates spin-glass (SG) ordering below $T_{\rm sg} = 23$K. Neutron scattering measurements indicate that the spin-glass behavior is associated with short-range spin density wave (SDW) ordering characterized by a static component and a low-energy dynamic component with a characteristic incommensurate wave vector of ${\bf Q}_m = (0.46, 0, 0.50)$ and an anisotropy gap of $\sim$ 2.5 meV. Our high ${\bf Q}$-resolution data also show that the systems undergo a glassy structural distortion that coincides with the short-range SDW order.
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Submitted 23 March, 2010;
originally announced March 2010.
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The local atomic structure of superconducting Fe-Se-Te
Authors:
Martin C. Lehman,
Despina Louca,
Kazumasa Horigane,
Anna Llobet,
Ryotaro Arita,
Sungdae Ji,
Naoyuki Katayama,
Shun Konbu,
Kazuma Nakamura,
Peng Tong,
Tae-Yeong Koo,
Kazuyoshi Yamada
Abstract:
We report on the first local atomic structure study via the pair density function (PDF) analysis of neutron diffraction data and show a direct correlation of local coordinates to TC in the newly discovered superconducting FeSe1-xTex. The isovalent substitution of Te for Se such as in FeSe0.5Te0.5 increases Tc by twofold in comparison to a-FeSe without changing the carrier concentration but, on a…
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We report on the first local atomic structure study via the pair density function (PDF) analysis of neutron diffraction data and show a direct correlation of local coordinates to TC in the newly discovered superconducting FeSe1-xTex. The isovalent substitution of Te for Se such as in FeSe0.5Te0.5 increases Tc by twofold in comparison to a-FeSe without changing the carrier concentration but, on average, decreases the chalcogen-Fe bond angle. However, we find that the local symmetry is lower than the average P4/nmm crystal symmetry, because the Se and Te ions do not share the same site, leading to two distinct z-coordinates that exhibit two types of bond angles with Fe. The angle indeed increases from ~ 104.02o in FeSe to ~105.20o in FeSe0.5Te0.5 between Fe and Se. Simultaneously, ab-initio calculations based on spin density function theory yielded an optimized structure with distinct z-coordinates for Se and Te, in agreement with the experiment. The valence charge distribution in the Fe-Se bonds was found to be different from that in the Fe-Te bonds. Thus, superconductivity in this chalcogenide is closely related to the local structural environment, with direct implications on the multiband magnetism where modulations of the ionic lattice can change the distribution of valence electrons.
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Submitted 2 September, 2009;
originally announced September 2009.
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Nano-magnetic droplets and implications to orbital ordering in La1-xSrxCoO3
Authors:
D. Phelan,
Despina Louca,
S. Rosenkranz,
S. -H. Lee,
Y. Qiu,
P. J. Chupas,
R. Osborn,
H. Zheng,
J. F. Mitchell,
J. R. D. Copley,
J. L. Sarrao,
Y. Moritomo
Abstract:
Inelastic cold neutron scattering on LaCoO3 provided evidence for a distinct low energy excitation at 0.6 meV coincident with the thermally induced magnetic transition. Coexisting strong ferromagnetic (FM) and weaker antiferromagnetic (AFM) correlations that are dynamic follow the activation to the excited state, identified as the intermediate S=1 spin triplet. This is indicative of dynamical or…
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Inelastic cold neutron scattering on LaCoO3 provided evidence for a distinct low energy excitation at 0.6 meV coincident with the thermally induced magnetic transition. Coexisting strong ferromagnetic (FM) and weaker antiferromagnetic (AFM) correlations that are dynamic follow the activation to the excited state, identified as the intermediate S=1 spin triplet. This is indicative of dynamical orbital ordering favoring the observed magnetic interactions. With hole doping as in La1-xSrxCoO3, the FM correlations between Co spins become static and isotropically distributed due to the formation of FM droplets. The correlation length and condensation temperature of these droplets increase rapidly with metallicity due to the double exchange mechanism.
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Submitted 1 December, 2005;
originally announced December 2005.
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Orbital and spin chains in ZnV2O4
Authors:
S. -H. Lee,
D. Louca,
H. Ueda,
S. Park,
T. J. Sato,
M. Isobe,
Y. Ueda,
S. Rosenkranz,
P. Zschack,
J. Iniguez,
R. Osborn
Abstract:
Our powder inelastic neutron scattering data indicate that \zvo is a system of spin chains that are three dimensionally tangled in the cubic phase above 50 K due to randomly occupied $t_{2g}$ orbitals of V$^{3+}$ ($3d^2$) ions. Below 50 K in the tetragonal phase, the chains become straight due to antiferro-orbital ordering. This is evidenced by the characteristic wave vector dependence of the ma…
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Our powder inelastic neutron scattering data indicate that \zvo is a system of spin chains that are three dimensionally tangled in the cubic phase above 50 K due to randomly occupied $t_{2g}$ orbitals of V$^{3+}$ ($3d^2$) ions. Below 50 K in the tetragonal phase, the chains become straight due to antiferro-orbital ordering. This is evidenced by the characteristic wave vector dependence of the magnetic structure factor that changes from symmetric to asymmetric at the cubic-to-tetragonal transition.
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Submitted 8 October, 2004; v1 submitted 21 December, 2003;
originally announced December 2003.
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Dynamical disorder of spin-induced Jahn-Teller orbitals with the insulator-metal transition in cobaltates
Authors:
Despina Louca,
J. L. Sarrao
Abstract:
Using elastic and inelastic neutron scattering, we investigated the evolution of the local atomic structure and lattice dynamics of La(1-x)Sr(x)CoO3 (x=0-0.5) as it crosses over with x from an insulator to a ferromagnetic metal (FMM). Our pair density function analysis indicates that in the paramagnetic insulating (PMI) phase for all x, spin activation of Co3+ ions induces local static Jahn-Tell…
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Using elastic and inelastic neutron scattering, we investigated the evolution of the local atomic structure and lattice dynamics of La(1-x)Sr(x)CoO3 (x=0-0.5) as it crosses over with x from an insulator to a ferromagnetic metal (FMM). Our pair density function analysis indicates that in the paramagnetic insulating (PMI) phase for all x, spin activation of Co3+ ions induces local static Jahn-Teller (JT) distortions. The size of the JT lattice increases almost linearly with x. However, in the FMM phase, static JT distortions are absent for x <= 30 %. This coincides with narrowing of hw=22 and 24 meV modes in the phonon spectrum in which we argue is due to localized dynamical JT fluctuations. For x > 30%, static JT distortions reappear along with broadening of the phonon modes because of weakened charge-lattice interactions.
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Submitted 27 August, 2003;
originally announced August 2003.
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Phonons from neutron powder diffraction
Authors:
D. A. Dimitrov,
D. Louca,
H. Röder
Abstract:
The spherically averaged structure function $\soq$ obtained from pulsed neutron powder diffraction contains both elastic and inelastic scattering via an integral over energy. The Fourier transformation of $\soq$ to real space, as is done in the pair density function (PDF) analysis, regularizes the data, i.e. it accentuates the diffuse scattering. We present a technique which enables the extracti…
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The spherically averaged structure function $\soq$ obtained from pulsed neutron powder diffraction contains both elastic and inelastic scattering via an integral over energy. The Fourier transformation of $\soq$ to real space, as is done in the pair density function (PDF) analysis, regularizes the data, i.e. it accentuates the diffuse scattering. We present a technique which enables the extraction of off-center phonon information from powder diffraction experiments by comparing the experimental PDF with theoretical calculations based on standard interatomic potentials and the crystal symmetry. This procedure (dynamics from powder diffraction(DPD)) has been successfully implemented for two systems, a simple metal, fcc Ni, and an ionic crystal, CaF$_{2}$. Although computationally intensive, this data analysis allows for a phonon based modeling of the PDF, and additionally provides off-center phonon information from powder neutron diffraction.
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Submitted 23 November, 1998; v1 submitted 4 November, 1998;
originally announced November 1998.