arXiv subjects

R. S. Perry

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

At least 37 records · Page 2Linked to original sources

arXiv2018

In-situ strain-tuning of the metal-insulator-transition of Ca$_{2}$RuO$_{4}$ in angle-resolved photoemission experiments

We report the evolution of the $k$-space electronic structure of lightly doped bulk Ca$_{2}$RuO$_{4}$ with uniaxial strain. Using ultrathin plate-like crystals, we achieve strain levels up to $-4.1\%$, sufficient to suppress the Mott phase and access the previously unexplored metallic state at low temperature. Angle-resolved photoemission experiments performed while tuning the uniaxial strain reveal that metallicity emerges from a marked redistribution of charge within the Ru $t_{2g}$ shell, accompanied by a sudden collapse of the spectral weight in the lower Hubbard band and the emergence of a well defined Fermi surface which is devoid of pseudogaps. Our results highlight the profound roles of lattice energetics and of the multiorbital nature of Ca$_{2}$RuO$_{4}$ in this archetypal Mott transition and open new perspectives for spectroscopic measurements.

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arXiv2018

Mott transition and collective charge pinning in electron doped Sr2IrO4

We studied the in-plane dynamic and static charge conductivity of electron doped Sr2IrO4 using optical spectroscopy and DC transport measurements. The optical conductivity indicates that the pristine material is an indirect semiconductor with a direct Mott-gap of 0.55 eV. Upon substitution of 2% La per formula unit the Mott-gap is suppressed except in a small fraction of the material (15%) where the gap survives, and overall the material remains insulating. Instead of a zero energy mode (or Drude peak) we observe a soft collective mode (SCM) with a broad maximum at 40 meV. Doping to 10% increases the strength of the SCM, and a zero-energy mode occurs together with metallic DC conductivity. Further increase of the La substitution doesn't change the spectral weight integral up to 3 eV. It does however result in a transfer of the SCM spectral weight to the zero-energy mode, with a corresponding reduction of the DC resistivity for all temperatures from 4 to 300 K. The presence of a zero-energy mode signals that at least part of the Fermi surface remains ungapped at low temperatures, whereas the SCM appears to be caused by pinning a collective frozen state involving part of the doped electrons.

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arXiv2018

Nuclear resonant scattering from 193Ir as a probe of the electronic and magnetic properties of iridates

The high brilliance of the modern synchrotron radiation sources facilitates experiments with high energy x-rays. In this Letter we report on Nuclear Resonance Scattering at the 73 keV nuclear level in 193Ir. The transitions between the hyperfine split levels show an exceptionally large E2/M1 multi-polarity mixing ratio combined with an increased sensitivity to certain changes in the hyperfine field direction compared to non-mixing transitions. The method opens a new way for probing local magnetic and electronic properties of correlated materials containing iridium and provides novel insights into their anisotropic magnetism. In particular, unexpected out-of-plane components of magnetic hyperfine fields and non-zero electric field gradients in Sr2IrO4 have been detected and attributed to the presence of strong spin-orbit interaction. Due to the high, 62% natural abundance of the 193Ir isotope, no isotopic enrichment of the samples is required, qualifying the method for a broad range of applications.

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arXiv2018

High-pressure insulator-to-metal transition in Sr$_3$Ir$_2$O$_7$ studied by x-ray absorption spectroscopy

High-pressure x-ray absorption spectroscopy was performed at the Ir $L_3$ and $L_2$ absorption edges of Sr$_3$Ir$_2$O$_7$. The branching ratio of white line intensities continuously decreases with pressure, reflecting a reduction in the angular part of the expectation value of the spin-orbit coupling operator, $\left\langle {\bf L} \cdot {\bf S} \right\rangle$. Up to the high-pressure structural transition at 53 GPa, this behavior can be explained within a single-ion model, where pressure increases the strength of the cubic crystal field, which suppresses the spin-orbit induced hybridization of $J_{\text{eff}} = 3/2$ and $e_g$ levels. We observe a further reduction of the branching ratio above the structural transition, which cannot be explained within a single-ion model of spin-orbit coupling and cubic crystal fields. This change in $\left\langle {\bf L} \cdot {\bf S} \right\rangle$ in the high-pressure, metallic phase of Sr$_3$Ir$_2$O$_7$ could arise from non-cubic crystal fields or a bandwidth-driven hybridization of $J_{\text{eff}}=1/2,\,3/2$ states, and suggests that the electronic ground state significantly deviates from the $J_{\text{eff}}=1/2$ limit.

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arXiv2017

Transverse acoustic phonon anomalies at intermediate wavevectors in MgV$_{2}$O$_{4}$

Magnetic spinels (with chemical formula $AX_{2}$O$_{4}$, with $X$ a 3$d$ transition metal ion) that also have an orbital degeneracy are Jahn-Teller active and hence possess a coupling between spin and lattice degrees of freedom. At high temperatures, MgV$_{2}$O$_{4}$ is a cubic spinel based on V$^{3+}$ ions with a spin $S$=1 and a triply degenerate orbital ground state. A structural transition occurs at T$_{OO}$=63 K to an orbitally ordered phase with a tetragonal unit cell followed by an antiferromagnetic transition of T$_{N}$=42 K on cooling. We apply neutron spectroscopy in single crystals of MgV$_{2}$O$_{4}$ to show an anomaly for intermediate wavevectors at T$_{OO}$ associated with the acoustic phonon sensitive to the shear elastic modulus $\left(C_{11}-C_{12}\right)/2$. On warming, the shear mode softens for momentum transfers near close to half the Brillouin zone boundary, but recovers near the zone centre. High resolution spin-echo measurements further illustrate a temporal broadening with increased temperature over this intermediate range of wavevectors, indicative of a reduction in phonon lifetime. A subtle shift in phonon frequencies over the same range of momentum transfers is observed with magnetic fields. We discuss this acoustic anomaly in context of coupling to orbital and charge fluctuations.

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arXiv2016

Pressure dependence of the structure and electronic properties of Sr3Ir2O7

We study the structural evolution of Sr$_3$Ir$_2$O$_7$ as a function of pressure using x-ray diffraction. At a pressure of 54 GPa at room temperature, we observe a first-order structural phase transition, associated with a change from tetragonal to monoclinic symmetry, and accompanied by a 4% volume collapse. Rietveld refinement of the high-pressure phase reveals a novel modification of the Ruddlesden-Popper structure, which adopts an altered stacking sequence of the perovskite bilayers. As the positions of the oxygen atoms could not be reliably refined from the data, we use density functional theory (local-density approximation+$U$+spin orbit) to optimize the crystal structure, and to elucidate the electronic and magnetic properties of Sr$_3$Ir$_2$O$_7$ at high pressure. In the low-pressure tetragonal phase, we find that the in-plane rotation of the IrO$_6$ octahedra increases with pressure. The calculations further indicate that a bandwidth-driven insulator-metal transition occurs at $\sim$20 GPa, along with a quenching of the magnetic moment. In the high-pressure monoclinic phase, structural optimization resulted in complex tilting and rotation of the oxygen octahedra, and strongly overlapping $t_{2g}$ and $e_g$ bands. The $t_{2g}$ bandwidth renders both the spin-orbit coupling and electronic correlations ineffectual in opening an electronic gap, resulting in a robust metallic state for the high-pressure phase of Sr$_3$Ir$_2$O$_7$.

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arXiv2016

Multiple metamagnetic quantum criticality in Sr$_3$Ru$_2$O$_7$

Bilayer strontium ruthenate Sr$_3$Ru$_2$O$_7$ displays pronounced non-Fermi liquid behavior at magnetic fields around 8 T, applied perpendicular to the ruthenate planes, which previously has been associated with an itinerant metamagnetic quantum critical end point (QCEP). We focus on the magnetic Grüneisen parameter $Γ_{\rm H}$, which is the most direct probe to characterize field-induced quantum criticality. We confirm quantum critical scaling due to a putative two-dimensional QCEP near 7.845(5) T, which is masked by two ordered phases A and B, identified previously by neutron scattering. In addition we find evidence for a QCEP at 7.53(2) T and determine the quantum critical regimes of both instabilities and the effect of their superposition.

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arXiv2015

The importance of XY anisotropy in Sr2IrO4 revealed by magnetic critical scattering experiments

The magnetic critical scattering in Sr$_2$IrO$_4$ has been characterized using X-ray resonant magnetic scattering (XRMS) both below and above the 3D antiferromagnetic ordering temperature, T$_{\text{N}}$. The order parameter critical exponent below T$_{\text{N}}$ is found to be β=0.195(4), in the range of the 2D XYh$_4$ universality class. Over an extended temperature range above T$_{\text{N}}$, the amplitude and correlation length of the intrinsic critical fluctuations are well described by the 2D Heisenberg model with XY anisotropy. This contrasts with an earlier study of the critical scattering over a more limited range of temperature which found agreement with the theory of the isotropic 2D Heisenberg quantum antiferromagnet, developed to describe the critical fluctuations of the conventional Mott insulator La$_2$CuO$_4$ and related systems. Our study therefore establishes the importance of XY anisotropy in the low-energy effective Hamiltonian of Sr$_2$IrO$_4$, the prototypical spin-orbit Mott insulator.

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arXiv2015

Evidence of quantum dimer excitations in Sr$_3$Ir$_2$O$_7$

The magnetic excitation spectrum in the bilayer iridate Sr$_3$Ir$_2$O$_7$ has been investigated using high-resolution resonant inelastic x-ray scattering (RIXS) performed at the iridium L$_3$ edge and theoretical techniques. A study of the systematic dependence of the RIXS spectrum on the orientation of the wavevector transfer, $\mathbf{Q}$, with respect to the iridium-oxide bilayer has revealed that the magnon dispersion is comprised of two branches well separated in energy and gapped across the entire Brillouin zone. Our results contrast with those of an earlier study which reported the existence of a single dominant branch. While these earlier results were interpreted as two overlapping modes within a spin-wave model of weakly coupled iridium-oxide planes, our results are more reminiscent of those expected for a system of weakly coupled dimers. In this latter approach the lower and higher energy modes find a natural explanation as those corresponding to transverse and longitudinal fluctuations, respectively. We have therefore developed a bond-operator theory which describes the magnetic dispersion in Sr$_3$Ir$_2$O$_7$ in terms of quantum dimer excitations. In our model dimerisation is produced by the leading Heisenberg exchange, $J_c$, which couples iridium ions in adjacent planes of the bilayer. The Hamiltonian also includes in plane exchange, $J$, as well as further neighbour couplings and relevant anisotropies. The bond-operator theory provides an excellent account of the dispersion of both modes, while the measured $\mathbf{Q}$ dependence of the RIXS intensities is in reasonable qualitative accord with the spin-spin correlation function calculated from the theory. We discuss our results in the context of the quantum criticality of bilayer dimer systems in the presence of anisotropic interactions derived from strong spin-orbit coupling.

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arXiv2015

Collapse of the Mott gap and emergence of a nodal liquid in lightly doped Sr$_2$IrO$_4$

Superconductivity in underdoped cuprates emerges from an unusual electronic state characterised by nodal quasiparticles and an antinodal pseudogap. The relation between this state and superconductivity is intensely studied but remains controversial. The discrimination between competing theoretical models is hindered by a lack of electronic structure data from related doped Mott insulators. Here we report the doping evolution of the Heisenberg antiferromagnet Sr$_2$IrO$_4$, a close analogue to underdoped cuprates. We demonstrate that metallicity emerges from a rapid collapse of the Mott gap with doping, resulting in lens-like Fermi contours rather than disconnected Fermi arcs as observed in cuprates. Intriguingly though, the emerging electron liquid shows nodal quasiparticles with an antinodal pseudogap and thus bares strong similarities with underdoped cuprates. We conclude that anisotropic pseudogaps are a generic property of two-dimensional doped Mott insulators rather than a unique hallmark of cuprate high-temperature superconductivity.

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arXiv2014

Field tunable spin density wave phases in Sr3Ru2O7

The conduction electrons in a metal experience competing interactions with each other and the atomic nuclei. This competition can lead to many types of magnetic order in metals. For example, in chromium the electrons order to form a spin-density-wave (SDW) antiferromagnetic state. A magnetic field may be used to perturb or tune materials with delicately balanced electronic interactions. Here we show that the application of a magnetic field can induce SDW magnetic order in a metal, where none exists in the absence of the field. We use magnetic neutron scattering to show that the application of a large (~8T) magnetic field to the metamagnetic perovskite metal Sr3Ru2O7 can be used to tune the material through two magnetically-ordered SDW states. The ordered states exist over relatively small ranges in field (<0.4T) suggesting that their origin is due to a new mechanism related to the electronic fine structure near the Fermi energy, possibly combined with the stabilising effect of magnetic fluctuations. The magnetic field direction is shown to control the SDW domain populations which naturally explains the strong resistivity anisotropy or electronic nematic behaviour observed in this material.

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arXiv2014

Thermal conductivity across the metal-insulator transition in single crystalline hyperkagome Na$_{3+x}$Ir$_3$O$_8$

The hyperkagome antiferromagnet Na$_{4}$Ir$_3$O$_8$ represents the first genuine candidate for the realisation of a three-dimensional quantum spin-liquid. It can also be doped towards a metallic state, thus offering a rare opportunity to explore the nature of the metal-insulator transition in correlated, frustrated magnets. Here we report thermodynamic and transport measurements in both metallic and weakly insulating single crystals down to 150 mK. While in the metallic sample the phonon thermal conductivity ($κ^{ph}$) is almost in the boundary scattering regime, in the insulating sample we find a large reduction $κ^{ph}$ over a very wide temperature range. This result can be ascribed to the scattering of phonons off nanoscale disorder or off the gapless magnetic excitations that are seen in the low-temperature specific heat. This works highlights the peculiarity of the metal-insulator transition in Na$_{3+x}$Ir$_3$O$_8$ and demonstrates the importance of the coupling between lattice and spin degrees of freedom in the presence of strong spin-orbit coupling.

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arXiv2014

Crystal field splitting in Sr$_{n+1}$Ir$_n$O$_{3n+1}$ ($n$ = 1, 2) iridates probed by x-ray Raman spectroscopy

Non-resonant Raman spectroscopy in the hard X-ray regime has been used to explore the electronic structure of the first two members of the Ruddlesden-Popper series Sr$_{n+1}$Ir$_n$O$_{3n+1}$ of iridates. By tuning the photon energy transfer around 530 eV we have been able to explore the oxygen K near edge structure with bulk sensitivity. The angular dependence of the spectra has been exploited to assign features in the 528-535 eV energy range to specific transitions involving the Ir 5d orbitals. This has allowed us to extract reliable values for both the t2g-eg splitting arising from the cubic component of the crystal field (10Dq), in addition to the splitting of the eg orbitals due to tetragonal distortions. The values we obtain are (3.8, 1.6) eV and (3.55, 1.9) eV for Sr$_2$IrO$_4$ and Sr$_3$Ir$_2$O$_7$, respectively.

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arXiv2014

Spin wave spectrum of the quantum ferromagnet on the pyrochlore lattice Lu2V2O7

Neutron inelastic scattering has been used to probe the spin dynamics of the quantum (S=1/2) ferromagnet on the pyrochlore lattice Lu2V2O7. Well-defined spin waves are observed at all energies and wavevectors, allowing us to determine the parameters of the Hamiltonian of the system. The data are found to be in excellent overall agreement with a minimal model that includes a nearest- neighbour Heisenberg exchange J = 8:22(2) meV and a Dzyaloshinskii-Moriya interaction (DMI) D =1:5(1) meV. The large DMI term revealed by our study is broadly consistent with the model developed by Onose et al. to explain the magnon Hall effect they observed in Lu2V2O7 [1], although our ratio of D=J = 0:18(1) is roughly half of their value and three times larger than calculated by ab initio methods [2].

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arXiv2014

Pressure study of nematicity and quantum criticality in Sr$_3$Ru$_2$O$_7$ for an in-plane field

We study the relationship between the nematic phases of Sr$_3$Ru$_2$O$_7$ and quantum criticality. At ambient pressure, one nematic phase is associated with a metamagnetic quantum critical end point (QCEP) when the applied magnetic field is near the \textit{c}-axis. We show, however, that this metamagnetic transition does not produce the same nematic signatures when the QCEP is reached by hydrostatic pressure with the field applied in the \textit{ab}-plane. Moreover, a second nematic phase, that is seen for field applied in the \textit{ab}-plane close to, but not right at, a second metamagnetic anomaly, persists with minimal change to the highest applied pressure, 16.55 kbar. Taken together our results suggest that metamagnetic quantum criticality may not be necessary for the formation of a nematic phase in Sr$_3$Ru$_2$O$_7$.

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arXiv2013

Study of the electronic nematic phase of Sr$_3$Ru$_2$O$_7$ with precise control of the applied magnetic field vector

We report a study of the magnetoresistivity of high purity Sr$_3$Ru$_2$O$_7$, in the vicinity of its electronic nematic phase. By employing a triple-axis (9/1/1T) vector magnet, we were able to precisely tune both the magnitude and direction of the in-plane component of the magnetic field (H$_\parallel$). We report the dependence of the resistively determined anisotropy on H$_\parallel$ in the phase, as well as across the wider temperature-field region. Our measurements reveal a high-temperature anisotropy which mimics the behaviour of fluctuations from the underlying quantum critical point, and suggest the existence of a more complicated phase diagram than previously reported.

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arXiv2012

Robustness of basal-plane antiferromagnetic order and the $J_{eff}=1/2$ state in single-layer iridate spin-orbit Mott insulators

The magnetic structure and electronic groundstate of the layered perovskite Ba2IrO4 have been investigated using x-ray resonant magnetic scattering (XRMS). Our results are compared with those for Sr2IrO4, for which we provide supplementary data on its magnetic structure. We find that the dominant, long-range antiferromagnetic order is remarkably similar in the two compounds, and that the electronic groundstate in Ba2IrO4, deduced from an investigation of the XRMS $L_3/L_2$ intensity ratio, is consistent with a $J_{eff}=1/2$ description. The robustness of these two key electronic properties to the considerable structural differences between the Ba and Sr analogues is discussed in terms of the enhanced role of the spin-orbit interaction in 5d transition metal oxides.

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arXiv2012

Electronic nematicity and its relation to quantum criticality in Sr_3Ru_2O_7 studied by thermal expansion

We report high-resolution measurements of the in-plane thermal expansion anisotropy in the vicinity of the electronic nematic phase in Sr$_3$Ru$_2$O$_7$ down to very low temperatures and in varying magnetic field orientation. For fields applied along the c-direction, a clear second-order phase transition is found at the nematic phase, with critical behavior compatible with the two-dimensional Ising universality class (although this is not fully conclusive). Measurements in a slightly tilted magnetic field reveal a broken four-fold in-plane rotational symmetry, not only within the nematic phase, but extending towards slightly larger fields. We also analyze the universal scaling behavior expected for a metamagnetic quantum critical point, which is realized outside the nematic region. The contours of the magnetostriction suggest a relation between quantum criticality and the nematic phase.

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