arXiv subjects

A. S. Gibbs

Publications and source records attributed to A. S. Gibbs.

16 recordsLinked to original sources

arXiv2026

Directional Andreev-Reflection Signatures of Inter-Orbital Pairing in Sr$_2$RuO$_4$

Unconventional superconductivity in quasi--two-dimensional systems is commonly identified through the emergence of Andreev bound states (ABS) at in-plane edges, while surfaces perpendicular to out-of-plane direction remain fully gapped due to weak interlayer coherence. This directional anisotropy has long served as a key paradigm for constraining pairing symmetries. Here, we show that Sr$_2$RuO$_4$ exhibits a striking reversal of this behavior. Using edge- and surface-sensitive spectroscopy, we observe pronounced in-gap ABS at surfaces perpendicular to the out-of-plane direction, whereas in-plane edges exhibit a reduced intensity of the in-gap spectral features. We show that this anomalous anisotropy can arise from the inter-orbital character of the superconducting pairing. Both even- and odd-parity inter-orbital pairing channels naturally generate robust surface ABS while suppressing planar edge modes and can also provide a mechanism for the appearance of a horizontal line node. Supported by \textit{ab initio} and model calculations, including Sr$_2$RuO$_4$/Ag interface reconstructions, our results highlight the possible role of inter-orbital correlations in shaping the spectroscopic response and provide constraints on the structure of the superconducting order parameter in Sr$_2$RuO$_4$.

cond-mat.supr-con↗

arXiv2024

Metastable ordered states induced by low temperature annealing of δ-Ag2/3V2O5

In δ-Ag2/3V2O5 with charge degrees of freedom in V, it is known that the charge ordering state and physical properties of V that appear at low temperatures depend strongly on the ordering state of Ag. In this study, we focused on the Ag ions in the interlayer and studied the structure using synchrotron radiation powder diffraction in dependence on temperature. We found that when the sample is slowly cooled from room temperature and ordering occurs at the Ag sites, V4+/V5+ charge ordering of V and subsequent V4+-V4+ structural dimers are produced. Although quenching the sample from room temperature suppresses the ordering of Ag, annealing at around 160 K promotes partial ordering of Ag and allows a metastable phase to be realized. This metastable phase is maintained even when the temperature is lowered again, producing a remarkable change in low-temperature properties. These results indicate that the ordered state of Ag, which is the key to control the charge-ordered state and physical properties, can be controlled by low-temperature annealing. The results of this study may provide a methodology for the realization of metastable states in a wide range of material groups of vanadium compounds, where competition among various charge ordered states underlies the physical properties.

cond-mat.str-el↗

arXiv2023

The crystal and magnetic structure of cesium superoxide

CsO2 is a member of the family of alkali superoxides (formula AO2 with A= Na, K, Rb and Cs) that exhibit magnetic behavior arising from open $p$-shell electrons residing on O2- molecules. We use neutron diffraction to solve the crystal and magnetic structures of CsO2, and observe a complex series of structures on cooling from room temperature to 1.6 K. These include an incommensurate modulation along the a-axis of the structure at intermediate temperatures, which then locks into a commensurate modulation that doubles the unit cell compared to the previously supposed orthorhombic unit cell. In both incommensurate and commensurate phases our structural solution involves a staggering of the cesium ion positions along the b-axis, in contrast to studies of other alkali superoxides in which staggered tilts of the O2- dimers relative to the c-axis are seen. Below T ~ 10 K we observe magnetic Bragg reflections arising from an antiferromagnetically ordered structure with a wavevector of k = (0,0,0) (relative to the doubled crystallographic unit cell), with moments that point predominantly along the b-axis with a small component along the a-axis that hints at possible anisotropic exchange coupling (consistent with the crystal structure). Measurements of the magnetic Bragg reflections in an applied magnetic field suggest a spin-flop transition takes place between 2 T and 4 T in which moments likely flop to point along the crystallographic a-axis. Our measurements indicate that CsO2 is an interesting example of magnetic properties being inherently linked to the crystal structure, in that the staggered displacement of the cesium ions activates antisymmetric exchange which then permits the observed spin canting.

cond-mat.str-el↗

arXiv2022

Competing spin-orbital singlet states in the 4$d^4$ honeycomb ruthenate Ag$_3$LiRu$_2$O$_6$

When spin-orbit-entangled $d$-electrons reside on a honeycomb lattice, rich quantum states are anticipated to emerge, as exemplified by the $d^5$ Kitaev materials. Distinct yet equally intriguing physics may be realized with a $d$-electron count other than $d^5$. We found that the layered ruthenate Ag$_3$LiRu$_2$O$_6$ with $d^4$ Ru$^{4+}$ ions at ambient pressure forms a honeycomb lattice of spin-orbit-entangled singlets, which is a playground for frustrated excitonic magnetism. Under pressure, the singlet state does not develop the expected excitonic magnetism but experiences two successive transitions to other nonmagnetic phases, first to an intermediate phase with moderate distortion of honeycomb lattice, and eventually to a high-pressure phase with very short Ru-Ru dimer bonds. While the strong dimerization in the high-pressure phase originates from a molecular orbital formation as in the sister compound Li$_2$RuO$_3$, the intermediate phase represents a spin-orbit-coupled $J$-dimer state which is stabilized by the admixture of upper-lying $J_{\rm eff} = 1$-derived states. We argue that the $J$-dimer state is induced by a pseudo-Jahn-Teller effect associated with the low-lying spin-orbital excited states and is unique to spin-orbit-entangled $d^4$ systems. The discovery of competing singlet phases demonstrates rich spin-orbital physics of $d^4$ honeycomb compounds and paves the way for realization of unconventional magnetism.

cond-mat.str-el↗

arXiv2021

Formation of orbital molecules on a pyrochlore lattice induced by A-O bond covalency

The pyrochlore ruthenate In$_2$Ru$_2$O$_7$ displays a subtle competition between spin-orbital entanglement and molecular orbital formation. At room temperature, a spin-orbit-entangled singlet state was identified. With decreasing temperature, In$_2$Ru$_2$O$_7$ undergoes multiple structural transitions and eventually forms a nonmagnetic ground state with semi-isolated Ru$_2$O units on the pyrochlore lattice. The dominant hopping through the Ru-O-Ru linkage leads to molecular orbital formation within the Ru$_2$O units. This molecular orbital formation is unique in that it involves the O$^{2-}$ anions, unlike the transition-metal dimers observed in systems with edge-sharing octahedra. We argue that the covalent character of In-O bonds plays a pivotal role in the structural transitions and molecular orbital formation and such bonding character of "$A$-site" ions is an important ingredient for electronic phase competition in complex transition metal oxides.

cond-mat.str-el↗

arXiv2020

High sensitivity heat capacity measurements on Sr2RuO4 under uniaxial pressure

A key question regarding the unconventional superconductivity of Sr$_2$RuO$_4$ remains whether the order parameter is single- or two-component. Under a hypothesis of two-component superconductivity, uniaxial pressure is expected to lift their degeneracy, resulting in a split transition. The most direct and fundamental probe of a split transition is heat capacity. Here, we report development of new high-frequency methodology for measurement of heat capacity of samples subject to large and highly homogeneous uniaxial pressure. We place an upper limit on the heat capacity signature of any second transition of a few per cent of the primary superconducting transition. The normalized jump in heat capacity, $ΔC/C$, grows smoothly as a function of uniaxial pressure, but we find no qualitative evidence of a pressure-induced order parameter transition. Thanks to the high precision of our measurements, these findings place stringent constraints on theories of the superconductivity of Sr$_2$RuO$_4$.

cond-mat.supr-con↗

arXiv2019

High-resolution photoemission on Sr2RuO4 reveals correlation-enhanced effective spin-orbit coupling and dominantly local self-energies

We explore the interplay of electron-electron correlations and spin-orbit coupling in the model Fermi liquid Sr2RuO4 using laser-based angle-resolved photoemission spectroscopy. Our precise measurement of the Fermi surface confirms the importance of spin-orbit coupling in this material and reveals that its effective value is enhanced by a factor of about two, due to electronic correlations. The self-energies for the $β$ and $γ$ sheets are found to display significant angular dependence. By taking into account the multi-orbital composition of quasiparticle states, we determine self-energies associated with each orbital component directly from the experimental data. This analysis demonstrates that the perceived angular dependence does not imply momentum-dependent many-body effects, but arises from a substantial orbital mixing induced by spin-orbit coupling. A comparison to single-site dynamical mean-field theory further supports the notion of dominantly local orbital self-energies, and provides strong evidence for an electronic origin of the observed non-linear frequency dependence of the self-energies, leading to `kinks' in the quasiparticle dispersion of Sr2RuO4.

cond-mat.str-el↗

arXiv2018

Pressure-induced collapse of spin-orbital Mott state in the hyperhoneycomb iridate $β$-Li$_2$IrO$_3$

Hyperhoneycomb iridate $β$-Li$_2$IrO$_3$ is a three-dimensional analogue of two-dimensional honeycomb iridates, such as $α$-Li$_2$IrO$_3$, which recently appeared as another playground for the physics of Kitaev-type spin liquid. $β$-Li$_2$IrO$_3$ shows a non-collinear spiral ordering of spin-orbital-entangled $J_{\rm eff}$ = 1/2 moments at low temperature, which is known to be suppressed under a pressure of $\sim$2 GPa. With further increase of pressure, a structural transition is observed at $P_{\rm S}$ $\sim$ 4 GPa at room temperature. Using the neutron powder diffraction technique, the crystal structure in the high-pressure phase of $β$-Li$_2$IrO$_3$ above $P_{\rm S}$ was refined, which indicates the formation of Ir$_2$ dimers on the zig-zag chains, with the Ir-Ir distance even shorter than that of metallic Ir. We argue that the strong dimerization stabilizes the bonding molecular orbital state comprising the two local $d_{zx}$-orbitals on the Ir-O$_2$-Ir bond plane, which conflicts with the equal superposition of $d_{xy}$-, $d_{yz}$- and $d_{zx}$- orbitals in the $J_{\rm eff}$ = 1/2 wave function produced by strong spin-orbit coupling. The results of resonant inelastic x-ray scattering (RIXS) measurements and the electronic structure calculations are fully consistent with the collapse of the $J_{\rm eff}$ = 1/2 state. A subtle competition of various electronic phases is universal in honeycomb-based Kitaev materials.

cond-mat.str-el↗

arXiv2018

Magnetic interactions in PdCrO$_2$ and their effects on its magnetic structure

We report a neutron scattering study of the metallic triangular lattice antiferromagnet PdCrO$_2$. Powder neutron diffraction measurements confirm that the crystalline space group symmetry remains $R\bar{3}m$ below $T_N$. This implies that magnetic interactions consistent with the crystal symmetry do not stabilise the non-coplanar magnetic structure which was one of two structures previously proposed on the basis of single crystal neutron diffraction measurements. Inelastic neutron scattering measurements find two gaps at low energies which can be explained as arising from a dipolar-type exchange interaction. This symmetric anisotropic interaction also stabilises a magnetic structure very similar to the coplanar magnetic structure which was also suggested by the single crystal diffraction study. The higher energy magnon dispersion can be modelled by linear spin wave theory with exchange interactions up to sixth nearest-neighbors, but discrepancies remain which hint at additional effects unexplained by the linear theory.

cond-mat.str-el↗

arXiv2017

Robust Bain distortion in the premartensite phase of platinum substituted Ni2MnGa magnetic shape memory alloy

The premartensite phase of shape memory and magnetic shape memory alloys (MSMAs) is believed to be a precursor state of the martensite phase with preserved austenite phase symmetry. The thermodynamic stability of the premartensite phase and its relation to the martensitic phase is still an unresolved issue, even though it is critical to the understanding of the functional properties of MSMAs. We present here unambiguous evidence for macroscopic symmetry breaking leading to robust Bain distortion in the premartensite phase of 10% Pt substituted Ni2MnGa. We show that the robust Bain distorted premartensite (T2) phase results from another premartensite (T1) phase with preserved cubic-like symmetry through an isostructural phase transition. The T2 phase finally transforms to the martensite phase with additional Bain distortion on further cooling. Our results demonstrate that the premartensite phase should not be considered as a precursor state with the preserved symmetry of the cubic austenite phase.

cond-mat.mtrl-sci↗

arXiv2016

Strain Control of Fermiology and Many-Body Interactions in Two-Dimensional Ruthenates

Here we demonstrate how the Fermi surface topology and quantum many-body interactions can be manipulated via epitaxial strain in the spin-triplet superconductor Sr$_2$RuO$_4$ and its isoelectronic counterpart Ba$_2$RuO$_4$ using oxide molecular beam epitaxy (MBE), \emph{in situ} angle-resolved photoemission spectroscopy (ARPES), and transport measurements. Near the topological transition of the $γ$ Fermi surface sheet, we observe clear signatures of critical fluctuations, while the quasiparticle mass enhancement is found to increase rapidly and monotonically with increasing Ru-O bond distance. Our work demonstrates the possibilities for using epitaxial strain as a disorder-free means of manipulating emergent properties, many-body interactions, and potentially the superconductivity in correlated materials.

cond-mat.supr-con↗

arXiv2015

S=1/2 quantum critical spin ladders produced by orbital ordering in Ba2CuTeO6

The ordered hexagonal perovskite Ba2CuTeO6 hosts weakly coupled S=1/2 spin ladders produced by an orbital ordering of Cu2+. The magnetic susceptibility chi(T) of Ba2CuTeO6 is well described by that expected for isolated spin ladders with exchange coupling of J~86 K but shows a deviation from the expected thermally activated behavior at low temperatures below T*~25 K. An anomaly in chi(T), indicative of magnetic ordering, is observed at T_mag=16 K. No clear signature of long-range ordering, however, is captured in NMR, specific heat or neutron diffraction measurements at and below T_mag. The marginal magnetic transition, indicative of strong quantum fluctuations, is evidence that Ba2CuTeO6 is in very close proximity to a quantum critical point between a magnetically ordered phase and a gapped spin liquid controlled by inter-ladder couplings.

cond-mat.str-el↗

arXiv2015

An intermediate state between the kagome-ice and the fully polarized state in Dy$_2$Ti$_2$O$_7$

Dy$_2$Ti$_2$O$_7$ is at present the cleanest example of a spin-ice material. Previous theoretical and experimental work on the first-order transition between the kagome-ice and the fully polarized state has been taken as a validation for the dipolar spin-ice model. Here we investigate in further depth this phase transition using ac-susceptibility and dc-magnetization, and compare this results with Monte-Carlo simulations and previous magnetization and specific heat measurements. We find signatures of an intermediate state between the kagome-ice and full polarization. This signatures are absent in current theoretical models used to describe spin-ice materials.

cond-mat.stat-mech↗

arXiv2014

Muon-spin rotation measurements of the vortex state in Sr$_2$RuO$_4$: type-1.5 superconductivity, vortex clustering and a crossover from a triangular to a square vortex lattice

Muon-spin rotation has been used to probe vortex state in Sr$_2$RuO$_4$. At moderate fields and temperatures a lattice of triangular symmetry is observed, crossing over to a lattice of square symmetry with increasing field and temperature. At lower fields it is found that there are large regions of the sample that are completely free from vortices which grow in volume as the temperature falls. Importantly this is accompanied by {\it increasing} vortex density and increasing disorder within the vortex-cluster containing regions. Both effects are expected to result from the strongly temperature-dependent long-range vortex attractive forces arising from the multi-band chiral-order superconductivity.

cond-mat.supr-con↗

arXiv2010

Unconventional magnetization processes and thermal runaway in spin-ice Dy$_2$Ti$_2$O$_7$

We investigate the non-equilibrium behavior of the spin-ice material Dy$_2$Ti$_2$O$_7$ by studying its magnetization as a function of the rate at which an external field is swept. At temperatures below the enigmatic "freezing" temperature $T_{\rm equil}\approx600$ mK, we find that even the slowest sweeps fail to yield the equilibrium magnetization curve and instead give a smooth, initially much flatter curve. For higher sweep rates, the magnetization develops sharp steps accompanied by similarly sharp peaks in the temperature of the sample. We ascribe the former behavior to the energy barriers encountered in the magnetization process, which proceeds via flipping of spins on filaments traced out by the field-driven motion of the gapped, long-range interacting magnetic monopole excitations. In contrast, the peaks in temperature result from the released Zeeman energy not being carried away efficiently into the bath, with the resulting heating triggering a chain reaction.

cond-mat.mtrl-sci↗

arXiv2010

Quantum oscillations near the metamagnetic transition in Sr3Ru2O7

We report detailed investigation of quantum oscillations in Sr3Ru2O7, observed inductively (the de Haas-van Alphen effect) and thermally (the magnetocaloric effect). Working at fields from 3 T to 18 T allowed us to straddle the metamagnetic transition region and probe the low- and high-field Fermi liquids. The observed frequencies are strongly field-dependent in the vicinity of the metamagnetic transition, and there is evidence for magnetic breakdown. We also present the results of a comprehensive rotation study. The most surprising result concerns the field dependence of the measured quasiparticle masses. Contrary to conclusions previously drawn by some of us as a result of a study performed with a much poorer signal to noise ratio, none of the five Fermi surface branches for which we have good field-dependent data gives evidence for a strong field dependence of the mass. The implications of these experimental findings are discussed.

cond-mat.str-el↗