arXiv subjects

R. S. Perry

Publications and source records attributed to R. S. Perry.

At least 19 recordsLinked to original sources

arXiv2026

Raman magnon spectroscopy of local interactions and ground state selection in $\mathrm{Sr_2IrO_4}$

Competing and coupled spin and charge interactions in quantum materials lead to a variety of ordered states where local configurations preferentially influence the long-range order. When these interactions are finely balanced in energy, disorder and fluctuations play an outsized role. Raman scattering is particularly well-suited to revealing the underlying physics in such situations because of its sensitivity to local environments and ability to reveal overall symmetries. We perform angle-resolved Raman polarization measurements on single crystals of the correlated, layered magnet, \ce{Sr2IrO4}, where the Mott insulating ground state arises from strong spin-orbit coupling. We characterize the symmetries of both the phonon and magnon modes through comprehensive measurements in both the $ab$-plane and out-of-plane geometries from 10 to 700 cm$^{-1}$, and trace the evolution of these modes in both configurations to 12 GPa in a diamond anvil cell with perforated diamonds. Pressure does not significantly alter the lattice as the phonon modes shift linearly under compression, but at the same time the magnon modes become position dependent and spread over a range of wavenumbers. We attribute this magnetic heterogeneity to pressure-enhanced variations in the weak interlayer interactions, which may locally favor competing magnetic stacking configurations, and compare our experimental results to the predictions of linear spin wave calculations. Our results demonstrate that Raman-active magnons amplify $\mu$eV-scale interactions responsible for ground-state selection into easily measurable spectral changes.

cond-mat.other↗

arXiv2024

Fermi surface and pseudogap in highly doped Sr$_{2}$IrO$_{4}$

The fate of the Fermi surface in bulk electron-doped Sr$_{2}$IrO$_{4}$ remains elusive, as does the origin and extension of its pseudogap phase. Here, we use high-resolution angle-resolved photoelectron spectroscopy (ARPES) to investigate the electronic structure of Sr$_{2-x}$La$_{x}$IrO$_{4}$ up to $x=0.2$, a factor of two higher than in previous work. We find that the antinodal pseudogap persists up to the highest doping level, and thus beyond the sharp increase in Hall carrier density to $\simeq 1+x$ recently observed above $x^{*}\simeq 0.16$ [Y.-T. Hsu et al., Nature Physics 20, 1593 (2024)]. This suggests that doped iridates host a unique phase of matter in which a large Hall density coexists with an anisotropic pseudogap, breaking up the Fermi surface into disconnected arcs. The temperature boundary of the pseudogap is $T^{*}\simeq 200$ K for $x=0.2$, comparable to cuprates and to the energy scale of short range antiferromagnetic correlations in cuprates and iridates.

cond-mat.str-el↗

arXiv2023

The Lorenz ratio as a guide to scattering contributions to Planckian transport

In many physical situations in which many-body assemblies exist at temperature $T$, a characteristic quantum-mechanical time scale of approximately $\hbar/k_{B}T$ can be identified in both theory and experiment, leading to speculation that it may be the shortest meaningful time in such circumstances. When this behaviour is investigated by probing the scattering rate of strongly interacting electrons in metals, it is clear that in some cases only electron-electron scattering can be its cause, while in others it arises from high-temperature scattering of electrons from quantised lattice vibrations, i.e. phonons. In metallic oxides, which are among the most studied materials, analysis of electrical transport does not satisfactorily identify the relevant scattering mechanism at 'high' temperatures near room temperature. We employ a contactless optical method to measure thermal diffusivity in two Ru-based layered perovskites, Sr$_3$Ru$_2$O$_7$ and Sr$_2$RuO$_4$, and use the measurements to extract the dimensionless Lorenz ratio. By comparing our results to the literature data on both conventional and unconventional metals we show how the analysis of high-temperature thermal transport can both give important insight into dominant scattering mechanisms, and be offered as a stringent test of theories attempting to explain anomalous scattering.

cond-mat.str-el↗

arXiv2023

Spin-orbital correlations from complex orbital order in MgV$_{2}$O$_{4}$

MgV$_{2}$O$_{4}$ is a spinel based on magnetic V$^{3+}$ ions which host both spin ($S=1$) and orbital ($l_{eff}=1$) moments. Owing to the underlying pyrochlore coordination of the magnetic sites, the spins in MgV$_{2}$O$_{4}$ only antiferromagnetically order once the frustrating interactions imposed by the $Fd\overline{3}m$ lattice are broken through an orbitally-driven structural distortion at T$_{S}$ $\simeq$ 60 K. Consequently, a N\'eel transition occurs at T$_{N}$ $\simeq$ 40 K. Low temperature spatial ordering of the electronic orbitals is fundamental to both the structural and magnetic properties, however considerable discussion on whether it can be described by complex or real orbital ordering is ambiguous. We apply neutron spectroscopy to resolve the nature of the orbital ground state and characterize hysteretic spin-orbital correlations using x-ray and neutron diffraction. Neutron spectroscopy finds multiple excitation bands and we parameterize these in terms of a multi-level (or excitonic) theory based on the orbitally degenerate ground state. Meaningful for the orbital ground state, we report an "optical-like" mode at high energies that we attribute to a crystal-field-like excitation from the spin-orbital $j_{eff}$=2 ground state manifold to an excited $j_{eff}$=1 energy level. We parameterize the magnetic excitations in terms of a Hamiltonian with spin-orbit coupling and local crystalline electric field distortions resulting from deviations from perfect octahedra surrounding the V$^{3+}$ ions. We suggest that this provides compelling evidence for complex orbital order in MgV$_{2}$O$_{4}$. We then apply the consequences of this model to understand hysteretic effects in the magnetic diffuse scattering where we propose that MgV$_{2}$O$_{4}$ displays a high temperature orbital memory of the low temperature spin order.

cond-mat.str-el↗

arXiv2022

Strain control of a bandwidth-driven spin reorientation in Ca$_{3}$Ru$_{2}$O$_{7}$

The layered-ruthenate family of materials possess an intricate interplay of structural, electronic and magnetic degrees of freedom that yields a plethora of delicately balanced ground states. This is exemplified by Ca$_{3}$Ru$_{2}$O$_{7}$, which hosts a coupled transition in which the lattice parameters jump, the Fermi surface partially gaps and the spins undergo a $90^{\circ}$ in-plane reorientation. Here, we show how the transition is driven by a lattice strain that tunes the electronic bandwidth. We apply uniaxial stress to single crystals of Ca$_{3}$Ru$_{2}$O$_{7}$, using neutron and resonant x-ray scattering to simultaneously probe the structural and magnetic responses. These measurements demonstrate that the transition can be driven by externally induced strain, stimulating the development of a theoretical model in which an internal strain is generated self-consistently to lower the electronic energy. We understand the strain to act by modifying tilts and rotations of the RuO$_{6}$ octahedra, which directly influences the nearest-neighbour hopping. Our results offer a blueprint for uncovering the driving force behind coupled phase transitions, as well as a route to controlling them.

cond-mat.str-el↗

arXiv2022

The magnetic structure and field dependence of the cycloid phase mediating the spin reorientation transition in Ca$_3$Ru$_2$O$_7$

We report a comprehensive experimental investigation of the magnetic structure of the cycloidal phase in Ca$_3$Ru$_2$O$_7$, which mediates the spin reorientation transition, and establishes its magnetic phase diagram. In zero applied field, single-crystal neutron diffraction data confirms the scenario deduced from an earlier resonant x-ray scattering study: between $46.7$~K $< T < 49.0$~K the magnetic moments form a cycloid in the $a-b$ plane with a propagation wavevector of $(δ,0,1)$ with $δ\simeq 0.025$ and an ordered moment of about 1 $μ_{\rm{B}}$, with the eccentricity of the cycloid evolving with temperature. In an applied magnetic field applied parallel to the $b$-axis, the intensity of the $(δ,0,1)$ satellite peaks decreases continuously up to about $μ_0 H \simeq 5$ T, above which field the system becomes field polarised. Both the eccentricity of the cycloid and the wavevector increase with field, the latter suggesting an enhancement of the anti$-$symmetric Dzyaloshinskii$-$Moriya interaction via magnetostriction effects. Transitions between the various low-temperature magnetic phases have been carefully mapped out using magnetometry and resistivity. The resulting phase diagram reveals that the cycloid phase exists in a temperature window that expands rapidly with increasing field, before transitioning to a polarised paramagnetic state at 5 T. High-field magnetoresistance measurements show that below $T\simeq 70$ K the resistivity increases continuously with decreasing temperature, indicating the inherent insulating nature at low temperatures of our high-quality, untwinned, single-crystals. We discuss our results with reference to previous reports of the magnetic phase diagram of Ca$_3$Ru$_2$O$_7$ that utilised samples which were more metallic and/or poly-domain.

cond-mat.str-el↗

arXiv2022

Quantum critical spin-liquid-like behavior in S = 1/2 quasikagome lattice CeRh1-xPdxSn investigated using muon spin relaxation and neutron scattering

We present the results of muon spin relaxation ($μ$SR) and neutron scattering on the Ce-based quasikagome lattice CeRh$_{1-x}$Pd$_{x}$Sn ($x=0.1$ to 0.75). Our ZF-$μ$SR results reveal the absence of static long-range magnetic order down to 0.05~K in $x = 0.1$ single crystals. The weak temperature-dependent plateaus of the dynamic spin fluctuations below 0.2~K in ZF-$μ$SR together with its longitudinal-field (LF) dependence between 0 and 3~kG indicate the presence of dynamic spin fluctuations persisting even at $T$ = 0.05~K without static magnetic order. On the other hand, $C_{\text{4f}}$/$T$ increases as --log $T$ on cooling below 0.9~K, passes through a broad maximum at 0.13~K and slightly decreases on further cooling. The ac-susceptibility also exhibits a frequency independent broad peak at 0.16~K, which is prominent with an applied field $H$ along $c$-direction. We, therefore, argue that such a behavior for $x=0.1$ (namely, a plateau in spin relaxation rate ($λ$) below 0.2~K and a linear $T$ dependence in $C_{\text{4f}}$ below 0.13~K) can be attributed to a metallic spin-liquid (SL) ground state near the quantum critical point in the frustrated Kondo lattice. The LF-$μ$SR study suggests that the out of kagome plane spin fluctuations are responsible for the SL behavior. Low energy inelastic neutron scattering (INS) of $x$ = 0.1 reveals gapless magnetic excitations, which are also supported by the behavior of $C_{\text{4f}}$ proportional to $T^{1.1}$ down to 0.06~K.

cond-mat.str-el↗

arXiv2022

Valence bond glass state in the 4$d^1$ fcc antiferromagnet Ba$_2$LuMoO$_6$

$B$-site ordered 4$d^1$ and 5$d^1$ double perovskites have a number of potential novel ground states including multipolar order, quantum spin liquids and valence bond glass states. These arise from the complex interactions of spin-orbital entangled $J_{eff}$ = 3/2 pseudospins on the geometrically frustrated fcc lattice. The 4$d^1$ Mo$^{5+}$ perovskite Ba$_2$YMoO$_6$ has been suggested to have a valence bond glass ground state. Here we report on the low temperature properties of powder samples of isostructural Ba$_2$LuMoO$_6$: the only other known cubic 4$d^1$ perovskite with one magnetic cation. Our muon spectroscopy experiments show that magnetism in this material remains dynamic down to 60 mK without any spin freezing or magnetic order. A singlet-triplet excitation with a gap of $Δ$ = 28 meV is observed in inelastic neutron scattering. These results are interpreted as a disordered valence bond glass ground state similar to Ba$_2$YMoO$_6$. Our results highlight the differences of the 4$d^1$ double perovskites in comparison to cubic 5$d^1$ analogues, which have both magnetic and multipolar order.

cond-mat.str-el↗

arXiv2021

Magnetic order, disorder, and excitations under pressure in the Mott insulator Sr$_2$IrO$_4$

Protected by the interplay of on-site Coulomb interactions and spin-orbit coupling, Sr$_2$IrO$_4$ at high pressure is a rare example of a Mott insulator with a paramagnetic ground state. Here, using optical Raman scattering, we measure both the phonon and magnon evolution in Sr$_2$IrO$_4$ under pressure, and identify three different magnetically-ordered phases, culminating in a spin-disordered state beyond 18 GPa. A strong first-order structural phase transition drives the magnetic evolution at $\sim$10 GPa with reduced structural anisotropy in the IrO$_6$ cages, leading to increasingly isotropic exchange interactions between the Heisenberg spins and a spin-flip transition to $c$-axis-aligned antiferromagnetic order. In the disordered phase of Heisenberg $J_\mathrm{eff}=1/2$ pseudospins, the spin excitations are quasi-elastic and continuous to 10 meV, potentially hosting a gapless quantum spin liquid in Sr$_2$IrO$_4$.

cond-mat.str-el↗

arXiv2021

Magnetic-field-controlled spin fluctuations and quantum criticality in Sr3Ru2O7

When the transition temperature of a continuous phase transition is tuned to absolute zero, new ordered phases and physical behaviour emerge in the vicinity of the resulting quantum critical point. Sr3Ru2O7 can be tuned through quantum criticality with magnetic field at low temperature. Near its critical field Bc it displays the hallmark T-linear resistivity and a T log(1/T) electronic heat capacity behaviour of strange metals. However, these behaviours have not been related to any critical fluctuations. Here we use inelastic neutron scattering to reveal the presence of collective spin fluctuations whose relaxation time and strength show a nearly singular variation with magnetic field as Bc is approached. The large increase in the electronic heat capacity and entropy near Bc can be understood quantitatively in terms of the scattering of conduction electrons by these spin-fluctuations. On entering the spin density wave (SDW) phase present near Bc, the fluctuations become stronger suggesting that the SDW order is stabilised through an "order-by-disorder" mechanism.

cond-mat.str-el↗

arXiv2021

Nodeless superconductivity in Lu$_{5-x}$Rh$_6$Sn$_{18+x}$ with broken time reversal symmetry

Evidence for broken time reversal symmetry (TRS) has been found in the superconducting states of the $R_5$Rh$_6$Sn$_{18}$ (R = Sc, Y, Lu) compounds with a centrosymmetric caged crystal structure, but the origin of this phenomenon is unresolved. Here we report neutron diffraction measurements of single crystals with $R$=Lu, as well as measurements of the temperature dependence of the magnetic penetration depth using a self-induced tunnel diode-oscillator (TDO) based technique, together with band structure calculations using density functional theory. Neutron diffraction measurements reveal that the system crystallizes in a tetragonal caged structure, and that one of nominal Lu sites in the Lu$_5$Rh$_6$Sn$_{18}$ structure is occupied by Sn, yielding a composition Lu$_{5-x}$Rh$_6$Sn$_{18+x}$ ($x=1$). The low temperature penetration depth shift $Δλ(T)$ exhibits an exponential temperature dependence below around $0.3T_c$, giving clear evidence for fully gapped superconductivity. The derived superfluid density is reasonably well accounted for by a single gap $s$-wave model, whereas agreement cannot be found for models of TRS breaking states with two-component order parameters. Moreover, band structure calculations reveal multiple bands crossing the Fermi level, and indicate that the aforementioned TRS breaking states would be expected to have nodes on the Fermi surface, in constrast to the observations.

cond-mat.supr-con↗

arXiv2020

Direct comparison of ARPES, STM, and quantum oscillation data for band structure determination in Sr$_2$RhO$_4$

Discrepancies in the low-energy quasiparticle dispersion extracted from angle resolved photoemission, scanning tunneling spectroscopy and quantum oscillation data are common and have long haunted the field of quantum matter physics. Here, we directly test the consistency of results from these three techniques by comparing data from the correlated metal Sr$_2$RhO$_4$. Using established schemes for the interpretation of the experimental data, we find good agreement for the Fermi surface topography and carrier effective masses. Hence, the apparent absence of such an agreement in other quantum materials, including the cuprates, suggests that the electronic states in these materials are of different, non-Fermi liquid like nature. Finally, we discuss the potential and challenges in extracting carrier lifetimes from photoemission and quasiparticle interference data.

cond-mat.str-el↗

arXiv2020

Spontaneous cycloidal order mediating a spin-reorientation transition in a polar metal

We show how complex modulated order can spontaneously emerge when magnetic interactions compete in a metal with polar lattice distortions. Combining neutron and resonant x-ray scattering with symmetry analysis, we reveal that the spin reorientation in Ca$_3$Ru$_2$O$_7$ is mediated by a magnetic cycloid whose eccentricity evolves smoothly but rapidly with temperature. We find the cycloid to be highly sensitive to magnetic fields, which appear to continuously generate higher harmonic modulations. Our results provide a unified picture of the rich magnetic phases of this correlated, multi-band polar metal.

cond-mat.str-el↗

arXiv2020

Correlated electron metal properties of the honeycomb ruthenate Na$_2$RuO$_3$

We report the synthesis and characterisation of polycrystalline Na$_2$RuO$_3$, a layered material in which the Ru$^{4+}$ ($4d^4$ configuration) form a honeycomb lattice. The optimal synthesis condition was found to produce a nearly ordered Na$_2$RuO$_3$ ($C2/c$ phase), as assessed from the refinement of the time-of-flight neutron powder diffraction. Magnetic susceptibility measurements reveal a large temperature-independent Pauli paramagnetism ($χ_0 \sim 1.42(2)\times10^{-3}$ emu/mol Oe) with no evidence of magnetic ordering down to 1.5 K, and with an absence of dynamic magnetic correlations, as evidenced by neutron scattering spectroscopy. The intrinsic susceptibility ($χ_0$) together with the Sommerfeld coeficient of $γ=11.7(2)$ mJ/Ru mol K$^2$ estimated from heat capacity measurements, gives an enhanced Wilson ratio of $R_W\approx8.9(1)$, suggesting that magnetic correlations may be present in this material. While transport measurements on pressed pellets show nonmetallic behaviour, photoemission spectrocopy indicate a small but finite density of states at the Fermi energy, suggesting that the bulk material is metallic. Except for resistivity measurements, which may have been compromised by near surface and interface effects, all other probes indicate that Na$_2$RuO$_3$ is a moderately correlated electron metal. Our results thus stand in contrast to earlier reports that Na$_2$RuO$_3$ is an antiferromagnetic insulator at low temperatures.

cond-mat.str-el↗

arXiv2019

Selective probing of magnetic order on Tb and Ir sites in stuffed Tb$_{2+x}$Ir$_{2-x}$O$_{7-y}$ using resonant X-ray scattering

We study the magnetic structure of the "stuffed" (Tb-rich) pyrochlore iridate Tb$_{2+x}$Ir$_{2-x}$O$_{7-y}$, using resonant elastic x-ray scattering (REXS). In order to disentangle contributions from Tb and Ir magnetic sublattices, experiments were performed at the Ir $L_3$ and Tb $M_5$ edges, which provide selective sensitivity to Ir $5d$ and Tb $4f$ magnetic moments, respectively. At the Ir $L_3$ edge, we found the onset of long-range ${\bf k}={\bf 0}$ magnetic order below $T_{N}^\text{Ir}\sim$ 71 K, consistent with the expected signal of all-in all-out (AIAO) magnetic order. Using a single-ion model to calculate REXS cross-sections, we estimate an ordered magnetic moment of $μ_{5d}^{\text{Ir}} \approx 0.34(3)\,μ_B$ at 5 K. At the Tb $M_5$ edge, long-range ${\bf k}={\bf 0}$ magnetic order appeared below $\sim40$ K, also consistent with an AIAO magnetic structure on the Tb site. Additional insight into the magnetism of the Tb sublattice is gleaned from measurements at the $M_5$ edge in applied magnetic fields up to 6 T, which is found to completely suppress the Tb AIAO magnetic order. In zero applied field, the observed gradual onset of the Tb sublattice magnetisation with temperature suggests that it is induced by the magnetic order on the Ir site. The persistence of AIAO magnetic order, despite the greatly reduced ordering temperature and moment size compared to stoichiometric Tb$_{2}$Ir$_{2}$O$_{7}$, for which $T_{N}^{\text{Ir}} =130$ K and $μ_{5d}^{\text{Ir}}=0.56\,μ_B$, indicates that stuffing could be a viable means of tuning the strength of electronic correlations, thereby potentially offering a new strategy to achieve topologically non-trivial band crossings in pyrochlore iridates.

cond-mat.str-el↗

arXiv2019

Momentum-resolved lattice dynamics of parent and electron-doped Sr$_{2}$IrO$_{4}$

The mixing of orbital and spin character in the wave functions of the $5d$ iridates has led to predictions of strong couplings among their lattice, electronic and magnetic degrees of freedom. As well as realizing a novel spin-orbit assisted Mott-insulating ground state, the perovskite iridate Sr$_{2}$IrO$_{4}$ has strong similarities with the cuprate La$_{2}$CuO$_{4}$, which on doping hosts a charge-density wave that appears intimately connected to high-temperature superconductivity. These phenomena can be sensitively probed through momentum-resolved measurements of the lattice dynamics, made possible by meV-resolution inelastic x-ray scattering. Here we report the first such measurements for both parent and electron-doped Sr$_{2}$IrO$_{4}$. We find that the low-energy phonon dispersions and intensities in both compounds are well described by the same nonmagnetic density functional theory calculation. In the parent compound, no changes of the phonons on magnetic ordering are discernible within the experimental resolution, and in the doped compound no anomalies are apparent due to charge-density waves. These measurements extend our knowledge of the lattice properties of (Sr$_{1-x}$La$_{x}$)$_{2}$IrO$_{4}$ and constrain the couplings of the phonons to magnetic and charge order.

cond-mat.str-el↗

arXiv2019

Critical fluctuations in the spin-orbit Mott insulator Sr$_3$Ir$_2$O$_7$

X-ray magnetic critical scattering measurements and specific heat measurements were performed on the perovskite iridate Sr$_3$Ir$_2$O$_7$. We find that the magnetic interactions close to the Néel temperature $T_N$ = 283.4(2) K are three-dimensional. This contrasts with previous studies which suggest two-dimensional behaviour like Sr$_2$IrO$_4$. Violation of the Harris criterion ($dν>2$) means that weak disorder becomes relevant. This leads a rounding of the antiferromagnetic phase transition at $T_N$, and modifies the critical exponents relative to the clean system. Specifically, we determine that the critical behaviour of Sr$_3$Ir$_2$O$_7$ is representative of the diluted 3D Ising universality class.

cond-mat.str-el↗

arXiv2019

Tuning of the Ru$^{\mathbf{4+}}$ ground-state orbital population in the $\mathbf{4d^4}$ Mott insulator Ca$_2$RuO$_4$ achieved by La doping

The ground-state orbital occupancy of the Ru$^{4+}$ ion in Ca$_{2-x}$La$_x$RuO$_4$ [x=0, 0.05(1), 0.07(1) and 0.12(1)] was investigated by performing X-ray absorption spectroscopy (XAS) in the vicinity of the O K edge as a function of angle between the incident beam and the surface of the crystals. A minimal model of the hybridization between the O 2p states probed at the K edge and the Ru 4d orbitals was used to analyze the XAS data, allowing the ratio of hole occupancies $n_{xy}/n_{yz,zx}$ to be determined as a function of doping and temperature. For the samples displaying a low-temperature insulating ground-state ($x\leq0.07$), $n_{xy}/n_{yz,zx}$ is found to increase significantly with increasing doping. For x=0.12, which has a metallic ground-state, the XAS spectra are found to be independent of temperature, and not to be describable by the minimal hybridization model. To understand the origin of the evolution of the electronic structure across the phase diagram, we have performed theoretical calculations based on a model Hamiltonian, comprising electron-electron correlations, crystal field ($Δ$) and spin-orbit coupling ($λ$), of a Ru-O-Ru cluster. Our calculations of the Ru hole occupancy as a function of $Δ/λ$ establish that the enhancement of $n_{xy}/n_{yz,zx}$ is driven by significant changes to the crystal field as the tetragonal distortion of the RuO$_6$ octahedral changes from compressive to tensile with La doping. It also shows that the hole occupancy of the O 2p and Ru 4d orbitals display the same trend as a function of $Δ/λ$, thus validating the minimal hybridization model. In essence, our results suggest that the predominant mechanism driving the emergence of the low-temperature metallic phase in La doped Ca$_2$RuO$_4$ is the structurally induced redistribution of holes within the t2g orbitals, rather that the injection of free carriers.

cond-mat.str-el↗