arXiv subjects

S. Calder

Publications and source records attributed to S. Calder.

At least 37 records · Page 2Linked to original sources

arXiv2019

Revisiting the Kitaev material candidacy of Ir4+ double perovskite iridates

Quantum magnets with significant bond-directional Ising interactions, so-called Kitaev materials, have attracted tremendous attention recently in the search for exotic spin liquid states. Here we present a comprehensive set of measurements that enables us to investigate the crystal structures, Ir$^{4+}$ single ion properties, and magnetic ground states of the double perovskite iridates La$_2B$IrO$_6$ ($B$ $=$ Mg, Zn) and $A_2$CeIrO$_6$ ($A$ $=$ Ba, Sr) with a large nearest neighbor distance $>$ 5 Angstroms between Ir$^{4+}$ ions. Our neutron powder diffraction data on Ba$_2$CeIrO$_6$ can be refined in the cubic space group Fm$\bar{3}$m, while the other three systems are characterized by weak monoclinic structural distortions. Despite the variance in the non-cubic crystal field experienced by the Ir$^{4+}$ ions in these materials, X-ray absorption spectroscopy and resonant inelastic x-ray scattering are consistent with $J_{\rm eff}$ $=$ 1/2 moments in all cases. Furthermore, neutron scattering and resonant magnetic x-ray scattering show that these systems host A-type antiferromagnetic order. These electronic and magnetic ground states are consistent with expectations for face-centered-cubic magnets with significant antiferromagnetic Kitaev exchange, which indicates that spacing magnetic ions far apart may be a promising design principle for uncovering additional Kitaev materials.

cond-mat.str-el↗

arXiv2019

Crossover from itinerant to localized magnetic excitations through the metal-insulator transition in NaOsO$_{\text{3}}$

NaOsO$_{\text{3}}$ undergoes a metal-insulator transition (MIT) at 410 K, concomitant with the onset of antiferromagnetic order. The excitation spectra have been investigated through the MIT by resonant inelastic x-ray scattering (RIXS) at the Os L$_{\text{3}}$ edge. Low resolution ($ΔE \sim$ 300 meV) measurements over a wide range of energies reveal that local electronic excitations do not change appreciably through the MIT. This is consistent with a picture in which structural distortions do not drive the MIT. In contrast, high resolution ($ΔE \sim $ 56 meV) measurements show that the well-defined, low energy magnons in the insulating state weaken and dampen upon approaching the metallic state. Concomitantly, a broad continuum of excitations develops which is well described by the magnetic fluctuations of a nearly antiferromagnetic Fermi liquid. By revealing the continuous evolution of the magnetic quasiparticle spectrum as it changes its character from itinerant to localized, our results provide unprecedented insight into the nature of the MIT in \naoso. In particular, the presence of weak correlations in the paramagnetic phase implies a degree of departure from the ideal Slater limit.

cond-mat.str-el↗

arXiv2019

Long range antiferromagnetic order in a rocksalt high entropy oxide

We report for the first time the magnetic structure of the high entropy oxide $(Mg_{0.2}Co_{0.2}Ni_{0.2}Cu_{0.2}Zn_{0.2})O$ using neutron powder diffraction. This material exhibits a sluggish magnetic transition but possesses a long-range ordered antiferromagnetic ground state, as revealed by DC and AC magnetic susceptibility, elastic and inelastic neutron scattering measurements. The magnetic propagation wavevector is k=(1/2, 1/2, 1/2) based on the cubic structure Fm-3m, and the magnetic structure consists of ferromagnetic sheets in the (111) planes with spins antiparallel between two neighboring planes. Inelastic neutron scattering reveals strong magnetic excitations at 100 K that survive up to room temperature. This work demonstrates that entropy-stabilized oxides represent a unique platform to study long range magnetic order with extreme chemical disorder.

cond-mat.mtrl-sci↗

arXiv2018

Magnetic excitations in the quasi-2D ferromagnet Fe3-xGeTe2 measured with inelastic neutron scattering

Fe3-xGeTe2 is an itinerant ferromagnet composed of two-dimensional layers weakly connected by van der Waals bonding that shows a variety of intriguing phenomena. Inelastic neutron scattering measurements on bulk single crystals of Fe2.75GeTe2 were performed to quantify the magnetic exchange interaction energies and anisotropy. The observed inelastic excitations are indicative of dominant in-plane correlations with negligible magnetic interactions between the layers. A spin-gap of 3.9 meV is observed allowing a measure of the magnetic anisotropy. As the excitations disperse to their maximum energy (~65 meV) they become highly damped, reflective of both the magnetic site occupancy reduction of 25{\%} on one Fe sublattice and the itinerant interactions. A minimal model is employed to describe the excitation spectra and extract nearest neighbor magnetic exchange interaction values. The temperature evolution of the excitations are probed and correlations shown to persist above Tc, indicative of low dimensional magnetism.

cond-mat.str-el↗

arXiv2018

Spin-gap and two-dimensional magnetic excitations in Sr2IrO4

Time-of-flight inelastic neutron scattering measurements on Sr2IrO4 single crystals were performed to access the spin Hamiltonian in this canonical Jeff=1/2 spin-orbital Mott insulator. The momentum of magnetic scattering at all inelastic energies that were measured is revealed to be $L$-independent, indicative of idealized two-dimensional in-plane correlations. By probing the in-plane energy and momentum dependence up to ~80 meV we model the magnetic excitations and define a spin-gap of 0.6(1) meV. Collectively the results indicate that despite the strong spin-orbit entangled isospins an isotropic two-dimensional S=1/2 Heisenberg model Hamiltonian accurately describes the magnetic interactions, pointing to a robust analogy with unconventional superconducting cuprates.

cond-mat.str-el↗

arXiv2018

Evolution of Magnetic and Orbital Properties in the Magnetically-Diluted A-Site Spinel Cu$_{1-x}$Zn$_x$Rh$_2$O$_4$

In frustrated spinel antiferromagnets, dilution with non-magnetic ions can be a powerful strategy for probing unconventional spin states or uncovering interesting phenomena. Here, we present X-ray, neutron scattering and thermodynamic studies of the effects of magnetic dilution of the tetragonally-distorted A-site spinel antiferromagnet, CuRh$_2$O$_4$, with non-magnetic Zn$^{2+}$ ions. Our data confirm the helical spin order recently identified at low-temperatures in this material, and further demonstrate a systematic suppression of the associated Néel temperature with increasing site dilution towards a continuous transition with critical doping of $x_{spin} \sim 0.44$. Interestingly, this critical doping is demonstrably distinct from a second structural critical point at $x_{JT} \sim 0.6$, which is consistent with the suppression of orbital order on the A-site through a classical percolative mechanism. This anomalously low value for $x_{spin}$ is confirmed via multiple measurements, and is inconsistent with predictions of classical percolation theory, suggesting that the spin transition in this material is driven by an enhancement of pre-existing spin fluctuations with weak dilution.

cond-mat.str-el↗

arXiv2018

Origin of magnetic excitation gap in double perovskite Sr$_2$FeOsO$_6$

Sr$_2$FeOsO$_6$ is an insulating double perovskite compound which undergoes antiferromagnetic transitions at 140 K ($T_{N1}$) and 67 K ($T_{N2}$). To study the underlying electronic and magnetic interactions giving rise to this behavior we have performed inelastic neutron scattering (INS) and resonant inelastic x-ray scattering (RIXS) experiments on polycrystalline samples of Sr$_2$FeOsO$_6$. The INS data reveal that the spectrum of spin excitations remains ungapped below T$_{N1}$, however below T$_{N2}$ a gap of 6.8 meV develops. The RIXS data reveals splitting of the T$_{2g}$ multiplet consistent with that seen in other 5d$^3$ osmium based double perovskites. Together these results suggest that spin-orbit coupling is important for ground state selection in 3d-5d$^3$ double perovskite materials.

cond-mat.str-el↗

arXiv2018

Negative thermal expansion and magnetoelastic coupling in the breathing pyrochlore lattice material LiGaCr4S8

The physical properties of the spinel LiGaCr4S8 have been studied with neutron diffraction, X-ray diffraction, magnetic susceptibility and heat capacity measurements. The neutron diffraction and synchrotron X-ray diffraction data reveal negative thermal expansion (NTE) below 111(4) K. The magnetic susceptibility deviates from Curie-Weiss behavior with the onset of NTE. At low temperature a broad peak in the magnetic susceptibility at 10.3(3) K is accompanied by the return of normal thermal expansion. First principles calculations find a strong coupling between the lattice and the simulated magnetic ground state. These results indicate strong magnetoelastic coupling in LiGaCr4S8.

cond-mat.other↗

arXiv2017

Interplay of spin-orbit coupling and hybridization in Ca3LiOsO6 and Ca3LiRuO6

The electronic ground state of Ca3LiOsO6 was recently considered within an intermediate coupling regime that revealed J=3/2 spin-orbit entangled magnetic moments. Through inelastic neutron scattering and density functional theory we investigate the magnetic interactions and probe how the magnetism is influenced by the change in hierarchy of interactions as we move from Ca3LiOsO6 (5d3) to Ca3LiRuO6 (4d3). An alteration of the spin-gap and ordered local moment is observed, however the magnetic structure, Neel temperature and exchange interactions are unaltered. To explain this behavior it is necessary to include both spin-orbit coupling and hybridization, indicating the importance of an intermediate coupling approach when describing 5$d$ oxides.

cond-mat.str-el↗

arXiv2017

Evidence for the Confinement of Magnetic Monopoles in Quantum Spin Ice

Magnetic monopoles are hypothesised elementary particles connected by Dirac strings that behave like infinitely thin solenoids. Despite decades of searches, free magnetic monopoles and their Dirac strings have eluded experimental detection, although there is substantial evidence for deconfined magnetic monopole quasiparticles in spin ice materials. Here we report the detection of a hierarchy of unequally-spaced magnetic excitations \emph{via} high resolution inelastic neutron spectroscopic measurements on the quantum spin ice candidate Pr$_{2}$Sn$_{2}$O$_{7}$. These excitations are well-described by a simple model of monopole pairs bound by a linear potential with an effective tension of 0.642(8) K~$\cdot$Å$^{-1}$ at 1.65~K. The success of the linear potential model suggests that these low energy magnetic excitations are direct spectroscopic evidence for the confinement of magnetic monopole quasiparticles in the quantum spin ice candidate Pr$_{2}$Sn$_{2}$O$_{7}$.

cond-mat.str-el↗

arXiv2017

Slater Insulator in Iridate Perovskites with Strong Spin-Orbit Coupling

The perovskite SrIrO3 is an exotic narrow-band metal owing to a confluence of the strengths of the spin-orbit coupling (SOC) and the electron-electron correlations. It has been proposed that topological and magnetic insulating phases can be achieved by tuning the SOC, Hubbard interactions, and/or lattice symmetry. Here, we report that the substitution of nonmagnetic, isovalent Sn4+ for Ir4+ in the SrIr1-xSnxO3 perovskites synthesized under high pressure leads to a metal-insulator transition to an antiferromagnetic (AF) phase at TN > 225 K. The continuous change of the cell volume as detected by x-ray diffraction and the lamda-shape transition of the specific heat on cooling through TN demonstrate that the metal-insulator transition is of second-order. Neutron powder diffraction results indicate that the Sn substitution enlarges an octahedral-site distortion that reduces the SOC relative to the spin-spin exchange interaction and results in the type-G AF spin ordering below TN. Measurement of high-temperature magnetic susceptibility shows the evolution of magnetic coupling in the paramagnetic phase typical of weak itinerant-electron magnetism in the Sn-substituted samples. A reduced structural symmetry in the magnetically ordered phase leads to an electron gap opening at the Brillouin zone boundary below TN in the same way as proposed by Slater.

cond-mat.str-el↗

arXiv2017

Tuning the antiferromagnetic helical pitch length and nanoscale domain size in Fe$_3$PO$_4$O$_3$ by magnetic dilution

The insulating magnetic material Fe3PO4O3 features a non-centrosymmetric lattice composed of Fe^{3+} triangular units. Frustration, due to competing near neighbor ($J_1$) and next nearest neighbor ($J_2$) antiferromagnetic interactions, was recently suggested to be the origin of an antiferromagnetic helical ground state with unusual needle-like nanoscale magnetic domains in Fe3PO4O3. Magnetic dilution is shown here to tune the ratio of these magnetic interactions, thus providing deeper insight into this unconventional antiferromagnet. Dilution of the Fe^{3+} lattice in Fe3PO4O3 was accomplished by substituting non-magnetic Ga^{3+} to form the solid solution series Fe_{3-x}Ga_xPO4O3 with $x = 0.012, 0.06, 0.25, 0.5, 1.0, 1.5$. Magnetic susceptibility and neutron powder diffraction data from this series are presented. A continuous decrease of the both the helical pitch length and the domain size is observed with increasing dilution up to at least $x = 0.25$, while for $x \ge 0.5$, the compounds lack long range magnetic order entirely. The decrease in the helical pitch length with increasing $x$ can be qualitatively understood by reduction of the ratio of $J_2/J_1$ in the Heisenberg model, consistent with mean field considerations. Intriguingly, the magnetic correlation length in the $ab$ plane remains nearly equal to the pitch length for each value of $x \le 0.25$, showing that the two quantities are intrinsically connected in this unusual antiferromagnet.

cond-mat.str-el↗

arXiv2017

Magnetic ground states and magnetodielectric effect in $R$Cr(BO$_3$)$_2$ ($R$ = Y and Ho)

The layered perovskites $R$Cr(BO$_3$)$_2$ ($R$ = Y and Ho) with magnetic triangular lattices were studied by performing ac/dc susceptibility, specific heat, elastic and inelastic neutron scattering, and dielectric constant measurements. The results show (i) both samples' Cr$^{3+}$ spins order in a canted antiferromagnetic structure with $T_N$ around 8-9 K, while the Ho$^{3+}$ ions do not order down to $T$ = 1.5 K in HoCr(BO$_3$)$_2$; (ii) when a critical magnetic field H$_{C}$ around 2-3 T is applied below $T_{N}$, the Cr$^{3+}$ spins in the Y-compound and both the Cr$^{3+}$ and Ho$^{3+}$ spins in the Ho-compound order in a ferromagnetic state; (iii) both samples exhibit dielectric constant anomalies around the transition temperature and critical field, but the Ho-compound displays a much stronger magnetodielectric response. We speculate that this is due to the magnetostriction which depends on both of the Cr$^{3+}$ and the Ho$^{3+}$ ions' ordering in the Ho-compound. Moreover, by using linear spin wave theory to simulate the inelastic neutron scattering data, we estimated the Y-compound's intralayer and interlayer exchange strengths as ferromagnetic J$_{1}$ = -0.12 meV and antiferromagnetic J$_{2}$ = 0.014 meV, respectively. The competition between different kinds of superexchange interactions results in the ferromagnetic intralayer interaction.

cond-mat.mtrl-sci↗

arXiv2017

Strongly Gapped Spin-Wave Excitation in the Insulating Phase of NaOsO3

NaOsO3 hosts a rare manifestation of a metal-insulator transition driven by magnetic correlations, placing the magnetic exchange interactions in a central role. We use resonant inelastic x-ray scattering to directly probe these magnetic exchange interactions. A dispersive and strongly gapped (58 meV) excitation is observed indicating appreciable spin-orbit coupling in this 5d3 system. The excitation is well described within a minimal model Hamiltonian with strong anisotropy and Heisenberg exchange (J1=J2=13.9 meV). The observed behavior places NaOsO3 on the boundary between localized and itinerant magnetism.

cond-mat.str-el↗

arXiv2017

Spin order and dynamics in the diamond-lattice Heisenberg antiferromagnets CuRh2O4 and CoRh2O4

Antiferromagnetic insulators on the diamond lattice are candidate materials to host exotic magnetic phenomena ranging from spin-orbital entanglement to degenerate spiral ground-states and topological paramagnetism. Compared to other three-dimensional networks of magnetic ions, such as the geometrically frustrated pyrochlore lattice, the investigation of diamond-lattice magnetism in real materials is less mature. In this work, we characterize the magnetic properties of model A-site spinels CoRh2O4 (cobalt rhodite) and CuRh2O4 (copper rhodite) by means of thermo-magnetic and neutron scattering measurements and perform group theory analysis, Rietveld refinement, mean-field theory, and spin wave theory calculations to analyze the experimental results. Our investigation reveals that cubic CoRh2O4 is a canonical S=3/2 diamond-lattice Heisenberg antiferromagnet with a nearest neighbor exchange J = 0.63 meV and a Neel ordered ground-state below a temperature of 25 K. In tetragonally distorted CuRh2O4, competiting exchange interactions between up to third nearest-neighbor spins lead to the development of an incommensurate spin helix at 24 K with a magnetic propagation vector k = (0,0,0.79). Strong reduction of the ordered moment is observed for the S=1/2 spins in CuRh2O4 and captured by our 1/S corrections to the staggered magnetization. Our work identifies CoRh2O4 and CuRh2O4 as reference materials to guide future work searching for exotic quantum behavior in diamond-lattice antiferromagnets.

cond-mat.str-el↗

arXiv2016

Strong anisotropy within a Heisenberg model in the J=1/2 insulating state of Sr2Ir0.8Ru0.2O4

The dispersive magnetic excitations in Sr2IrO4 have previously been well described within an isospin-1/2 Heisenberg model on a square lattice that revealed parallels with La2CuO4. Here we investigate the inelastic spectra of Sr2Ir0.8Ru0.2O4 with resonant inelastic x-ray scattering (RIXS) at the Ir L3-edge. The results are well described using linear spin-wave theory within a similar Heisenberg model applicable to Sr2IrO4, however the disorder induced by the substitution of 20% Ir4+ ions for Ru4+ removes longer range exchange interactions. A large spin-gap (40 meV) is measured indicating strong anisotropy from spin-orbit coupling that is manifest due to the altered magnetic structure in Sr2Ir0.8Ru0.2O4 with c-axis aligned moments compared to the basal plane moments in the parent. Collectively the results indicate the robustness of a Heisenberg model description even when the magnetic structure is altered and the J=1/2 moments diluted.

cond-mat.str-el↗

arXiv2016

Spin-orbit coupling controlled $J=3/2$ electronic ground state in 5$d^{3}$ oxides

Entanglement of spin and orbital degrees of freedom drives the formation of novel quantum and topological physical states. Discovering new spin-orbit entangled ground states and emergent phases of matter requires both experimentally probing the relevant energy scales and applying suitable theoretical models. Here we report resonant inelastic x-ray scattering measurements of the transition metal oxides Ca$_3$LiOsO$_6$ and Ba$_2$YOsO$_6$. We invoke an intermediate coupling approach that incorporates both spin-orbit coupling and electron-electron interactions on an even footing and reveal the ground state of $5d^3$ based compounds, which has remained elusive in previously applied models, is a novel spin-orbit entangled J=3/2 electronic ground state. This work reveals the hidden diversity of spin-orbit controlled ground states in 5d systems and introduces a new arena in the search for spin-orbit controlled phases of matter.

cond-mat.str-el↗

arXiv2016

Candidate Elastic Quantum Critical Point in LaCu$_{6-x}$Au$_x$

The structural properties of LaCu$_{6-x}$Au$_x$ have been studied using neutron diffraction, x-ray diffraction, and heat capacity measurements. The continuous orthorhombic-monoclinic structural phase transition in LaCu$_{6}$ is suppressed linearly with Au substitution until a complete suppression of the structural phase transition occurs at the critical composition, $x_{c}$ = 0.3. Heat capacity measurements at low temperatures indicate residual structural instability at $x_c$ that extends well into the orthorhombic phase. The instability is ferroelastic in nature, with density functional theory (DFT) calculations showing negligible coupling to electronic states near the Fermi level. The data and calculations presented here are consistent with the zero temperature termination of a continuous structural phase transition suggesting that the LaCu$_{6-x}$Au$_x$ series hosts an elastic quantum critical point.

cond-mat.str-el↗