arXiv subjects

Jeffrey A. Quilliam

Publications and source records attributed to Jeffrey A. Quilliam.

7 recordsLinked to original sources

arXiv2025

Superconducting meander-line surface coil for NMR spectroscopy of nanoscale thin films

Nuclear magnetic resonance (NMR) spectroscopy is a powerful technique to study local magnetism in a variety of materials. However, the inherently low sensitivity of conventional inductively detected solid state NMR typically requires a large number of spins, reducing its applicability to two-dimensional (2D) materials and nanoscale thin films. To overcome this experimental challenge, we introduce a novel probe based on a superconducting meander-line surface coil that significantly enhances the NMR sensitivity for thin samples. Using a NbN meander with an optimized geometry, we demonstrate the sensitivity of this technique by detecting the NMR signal of a 150-nm-thick boron film containing only $\sim 2\times10^{16}$ $^{11}$B nuclear spins. Spin-echo measurements and theoretical modeling offer insight into the parameters limiting the coil's performance. This work lays the foundation for developing highly sensitive NMR probes, potentially unlocking new opportunities for studying atomically thin materials.

cond-mat.mes-hall↗

arXiv2025

Dipolar-octupolar correlations and hierarchy of exchange interactions in Ce$_2$Hf$_2$O$_7$

High-resolution neutron spectroscopy on Ce$_2$Hf$_2$O$_7$ reveals a correlated state characterized by distinct dipolar scattering signals -- quasi-elastic and inelastic contributions consistent with `photon' and `spinon' excitations in quantum spin ice. These signals coexist with weak octupolar scattering. Fits of thermodynamic data using numerical methods indicate a dominant octupolar exchange, $J_{x}$ or $J_{y}$, with substantial dipolar $J_{z}$ and minute dipole-octupole $J_{xz}$ couplings. The $J_{xz}$ value is corroborated by an independent fit of the neutron scattering amplitude balance between dipolar and octupolar `photon' contributions, highlighting its importance to understand neutron scattering results in this family. Ce$_2$Hf$_2$O$_7$ enriches the landscape of dipole-octupole pyrochlore physics, and reveals a `quantum multipolar liquid' where hybrid correlations involve multiple terms in moment series expansion, opening questions on their intertwining and hierarchy in quantum phases.

cond-mat.str-el↗

arXiv2025

Thermodynamics of the dipole-octupole pyrochlore magnet Ce$_2$Hf$_2$O$_{7}$ in applied magnetic fields

The recently discovered dipole-octupole pyrochlore magnet Ce$_2$Hf$_2$O$_7$ is a promising three-dimensional quantum spin liquid candidate which shows no signs of ordering at low temperature. The low energy effective pseudospin-1/2 description in a magnetic field is characterized by the XYZ Hamiltonian and a Zeeman term where the dipolar local $z$-component of the pseudospin couples to the local $z$-component of the applied magnetic field, while the local $x$- and $y$-components of the pseudospin remain decoupled as a consequence of their octupolar character. Using effective Hamiltonian parameters determined in V. Poree et al., arXiv:2305.08261 (2023), remarkable experimental features can be reproduced, as for instance the specific heat and magnetization data as well as the continuum of states seen in neutron scattering. Here we investigate the thermodynamic response to magnetic fields applied along the global [110] direction using specific heat measurements and fits using numerical methods, and solve the corresponding magnetic structure using neutron diffraction. Specific heat data in moderate fields are reproduced well, however, at high fields the agreement is not satisfactory. We especially observe a two-step release of entropy, a finding that demands a review of both theory and experiment. We address it within the framework of three possible scenarios, including an analysis of the crystal field Hamiltonian not restricted to the two-dimensional single-ion doublet subspace. We conclusively rule out two of these scenarios and find qualitative agreement with a simple model of field misalignment with respect to the crystalline direction. We discuss the implications of our findings for [111] applied fields and for future experiments on Ce$_2$Hf$_2$O$_7$ and its sister compounds.

cond-mat.str-el↗

arXiv2024

Collapse of susceptibility and non-trivial spin dynamics in the hyper-honeycomb magnet $β$-Li$_2$IrO$_3$ under high pressure

We present high-pressure (2 GPa) $^7$Li nuclear magnetic resonance (NMR) measurements on single crystals of the hyper-honeycomb Kitaev magnet $β$-Li$_2$IrO$_3$. The spectra show evidence for a structural phase transition around 200 K and a coexistence of phases, consistent with the results of other measurement techniques. The NMR spectra and line shift measurements demonstrate a strong suppression of the local magnetic susceptibility at high pressure. However, the spin-lattice relaxation ($1/T_1$) shows a clear power-law temperature dependence. This is inconsistent with a gapped singlet ground state of dimers and tetramers, as was previously proposed, and is instead evocative of a more exotic quantum spin liquid-like ground state.

cond-mat.str-el↗

arXiv2024

Giant anisotropic magnetoresistance in few-layer α-RuCl3 tunnel junctions

The spin-orbit assisted Mott insulator $α$-RuCl3 is proximate to the coveted quantum spin liquid (QSL) predicted by the Kitaev model. In the search for the pure Kitaev QSL, reducing the dimensionality of this frustrated magnet by exfoliation has been proposed as a way to enhance magnetic fluctuations and Kitaev interactions. Here, we perform angle-dependent tunneling magnetoresistance (TMR) measurements on ultrathin $α$-RuCl3 crystals with various layer numbers to probe their magnetic, electronic and crystal structure. We observe a giant change in resistance - as large as ~2500% - when the magnetic field rotates either within or out of the $α$-RuCl3 plane, a manifestation of the strongly anisotropic spin interactions in this material. In combination with scanning transmission electron microscopy, this tunneling anisotropic magnetoresistance (TAMR) reveals that few-layer $α$-RuCl3 crystals remain in the high-temperature monoclinic phase at low temperature. It also shows the presence of a zigzag antiferromagnetic order below the critical temperature TN ~ 14 K, which is twice the one typically observed in bulk samples with rhombohedral stacking. Our work offers valuable insights into the relation between the stacking order and magnetic properties of this material, which helps lay the groundwork for creating and electrically probing exotic magnetic phases like QSLs via van der Waals engineering.

cond-mat.str-el↗

arXiv2024

The magnetic structure of Ce$_3$TiBi$_5$ and its relation to current-induced magnetization

The control of magnetization using electric fields has been extensively studied in magnetoelectric multiferroic insulator materials. Changes in magnetization in bulk metals caused by electric currents have attracted less attention. The recently discovered metallic magnet Ce$_3$TiBi$_5$ has been reported to exhibit current-induced magnetization. Here we determined the magnetic structure of Ce$_3$TiBi$_5$ using neutron diffraction, aiming to understand the microscopic origin of this magnetoelectric phenomenon in a metal. We established that the antiferromagnetic order emerging below $T_N=5$ K is a cycloid order described by $P6_3/mcm.1'(0,0,g)00sss$ with small moment sizes of $0.50(2)~μ_B$ and propagation vector ${\bf k}=(0,0,0.386)$. Surprisingly, the symmetry of this magnetic structure is inconsistent with the presence of current-induced magnetization and potential origins of this inconsistency with previous results are discussed. Additionally, our results suggest that moments order along their hard magnetic direction in Ce$_3$TiBi$_5$, a phenomenon which has been observed in other Kondo systems.

cond-mat.str-el↗

arXiv2022

Anticollinear order and degeneracy lifting in square lattice antiferromagnet LaSrCrO4

We report the static and dynamic magnetic properties of LaSrCrO$_4$, a seemingly canonical spin-3/2 square-lattice antiferromagnet that exhibits frustration between magnetic layers -- owing to their AB stacking -- and offers a rare testbed to investigate accidental-degeneracy lifting in magnetism. Neutron diffraction experiments on single-crystal samples uncover a remarkable anticollinear magnetic order below $T_N$ = 170 K characterized by a Néel arrangement of the spins within each layer and an orthogonal arrangement between adjacent layers. To understand the origin of this unusual magnetic structure, we analyze the spin-wave excitation spectrum by means of inelastic neutron scattering and bulk measurements. A spectral gap of 0.5 meV, along with a spin-flop transition at 3.2\, T, reflect the energy scale associated with the degeneracy-lifting. A minimal model to explain these observations requires both a positive biquadratic interlayer exchange and dipolar interactions, both of which are on the order of 10$^{-4}$ meV, only a few parts per million of the dominant exchange interaction $J_1 \approx 11$ meV. These results provide direct evidence for the selection of a non-collinear magnetic structure by the combined effect of two distinct degeneracy lifting interactions.

cond-mat.str-el↗