arXiv subjects

R. A. Mole

Publications and source records attributed to R. A. Mole.

14 recordsLinked to original sources

arXiv2026

The Magnetic Ground State of Atacamite Cu$_2$Cl(OH)$_3$: The Crucial Role of Frustrated Zigzag Chains Revealed by Inelastic Neutron Scattering

We report inelastic neutron scattering (INS) measurements on the magnetically frustrated $S=\frac12$ sawtooth-chain compound atacamite Cu$_2$Cl(OH)$_3$ featuring inequivalent Cu(1) and Cu(2) sites. Transverse to the sawtooth chains, INS reveals two dispersive spin-wave modes and a gap of at least 0.75 meV. This behavior is rationalized within a zigzag-chain model of Cu(2) spins in an effective magnetic field of Cu(1) spins. The model is compatible with first-principles calculations and accounts for INS dispersions within linear spin-wave theory calculations. Our results reveal a unique case of an effective separation of energy scales between two differently oriented one-dimensional chains, with the zigzag-chain model being essential to fully characterize atacamite's low-energy magnetism.

cond-mat.str-el↗

arXiv2023

Competing itinerant and local spin interactions in kagome metal FeGe

Two-dimensional kagome metals consisting of corner-sharing triangles offer a unique platform for studying strong electron correlations and band topology due to its geometrically frustrated lattice structure. The similar energy scales between spin, lattice, and electronic degrees of freedom in these systems give rise to competing quantum phases such as charge density wave (CDW), magnetic order, and superconductivity. For example, kagome metal FeGe first exhibits A-type collinear antiferromagnetic (AFM) order at T_N ~ 400 K, then establishes a CDW phase coupled with AFM ordered moment below T_CDW ~ 100 K, and finally forms a $c$-axis double cone AFM structure around T_Canting ~ 60 K. Here we use neutron scattering to demonstrate the presence of gapless incommensurate spin excitations associated with the double cone AFM structure at temperatures well above T_Canting and T_CDW that merge into gapped commensurate spin waves from the A-type AFM order. While commensurate spin waves follow the Bose population factor and can be well described by a local moment Heisenberg Hamiltonian, the incommensurate spin excitations first appear below T_N where AFM order is commensurate, start to deviate from the Bose population factor around T_CDW, and peaks at T_Canting, consistent with a critical scattering of a second order magnetic phase transition, as a function of decreasing temperature. By comparing these results with density functional theory calculations, we conclude that the incommensurate magnetic structure arises from the nested Fermi surfaces of itinerant electrons and the formation of a spin density wave order. The temperature dependence of the incommensurate spin excitations suggests a coupling between spin density wave and CDW order, likely due to flat electronic bands near the Fermi level around T_N and associated electron correlation effects.

cond-mat.str-el↗

arXiv2019

Does the boson peak survive in an ultrathin oxide glass?

Bulk glasses exhibit extra vibrational modes at low energies, known as the boson peak. The microscopic dynamics in nanoscale alumina impact the performance of qubits and other superconducting devices, however the existence of the boson peak in these glasses has not been previously measured. Here we report neutron spectroscopy on Al/Al$_2$O$_{3-x}$ nanoparticles consisting of spherical metallic cores from 20 to 1000 nm surrounded by a 3.5 nm thick alumina glass. An intense low-energy peak is observed at $ω_{BP}$ = 2.8 $\pm$ 0.6 meV for highly oxidised particles, concurrent with an excess in the density of states. The intensity of the peak scales inversely with particle size and oxide fraction indicating a surface origin, and is red-shifted by 3 meV with respect to the van-Hove singularity of $γ$-phase Al$_2$O$_{3-x}$ nanocrystals. Molecular dynamics simulations of $α$-Al$_2$O$_{3-x}$, $γ$-Al$_2$O$_{3-x}$ and a-Al$_2$O$_{3-x}$ show that the observed boson peak is a signature of the ultrathin glass surface, and the frequency is softened compared to that of the hypothetical bulk glass.

cond-mat.mtrl-sci↗

arXiv2017

Stability of charge-stripe ordered La2-xSrxNiO4+delta at one third doping

The stability of charge ordered phases is doping dependent, with different materials having particularly stable ordered phases. In the half filled charge ordered phases of the cuprates this occurs at one eighth doping, whereas in charge-stripe ordered La2-xSrxNiO4+delta there is enhanced stability at one third doping. In this paper we discuss the known details of the charge-stripe order in La2-xSrxNiO4+delta, and how these properties lead to the one third doping stability.

cond-mat.str-el↗

arXiv2017

Cluster-based Haldane state in edge-shared tetrahedral spin-cluster chain: Fedotovite K$_2$Cu$_3$O(SO$_4$)$_3$

Fedotovite K$_2$Cu$_3$O(SO$_4$)$_3$ is a candidate of new quantum spin systems, in which the edge-shared tetrahedral (EST) spin-clusters consisting of Cu$^{2+}$ are connected by weak inter-cluster couplings to from one-dimensional array. Comprehensive experimental studies by magnetic susceptibility, magnetization, heat capacity, and inelastic neutron scattering measurements reveal the presence of an effective $S$ = 1 Haldane state below $T \cong 4$ K. Rigorous theoretical studies provide an insight into the magnetic state of K$_2$Cu$_3$O(SO$_4$)$_3$: an EST cluster makes a triplet in the ground state and one-dimensional chain of the EST induces a cluster-based Haldane state. We predict that the cluster-based Haldene state emerges whenever the number of tetrahedra in the EST is $even$.

cond-mat.str-el↗

arXiv2017

Magnetic excitations of the charge stripe electrons below half doping in La(2-x)Sr(x)NiO4, x = 0.45 and x = 0.4

The low energy magnetic excitation spectrum of charge stripe ordered La(2-x)Sr(x)NiO4, x = 0.4 and x = 0.45 samples were studied by neutron scattering. Two excitation modes are observed in both materials, one from the ordered magnetic moments, and a second mode consistent with pseudo-one-dimensional antiferromagnetic excitations of the charge stripe electrons (q-1D). The dispersion of the q-1D excitation follows the same relation as in x = 1/3 composition, with even spectral weight in the two counter-propagating branches of the x = 0.4 sample, however in the $x = 0.45$ sample only one dispersion branch has any measurable spectral weight. The evolution of the q-1D excitations on doping to the checkerboard charge ordered phase is discussed.

cond-mat.str-el↗

arXiv2017

The dynamics of linarite: Observations of magnetic excitations

Here we present inelastic neutron scattering measurements from the frustrated, quantum spin-1/2 chain material linarite, PbCuSO_4(OH)_2. Time of flight data, taken at 0.5K and zero applied magnetic field reveals low-energy dispersive spin wave excitations below 1.5meV both parallel and perpendicular to the Cu-chain direction. From this we confirm that the interchain couplings within linarite are around 10% of the nearest neighbour intrachain interactions. We analyse the data within both linear spin-wave theory and density matrix renormalisation group theories and establish the main magnetic exchange interactions and the simplest realistic Hamiltonian for this material.

cond-mat.str-el↗

arXiv2016

Low-Energy Excitations and Ground State Selection in Quantum Breathing Pyrochlore Antiferromagnet Ba$_3$Yb$_2$Zn$_5$O$_{11}$

We study low energy excitations in the quantum breathing pyrochlore antiferromagnet Ba$_3$Yb$_2$Zn$_5$O$_{11}$ by combination of inelastic neutron scattering (INS) and thermodynamical properties measurements. The INS spectra are quantitatively explained by spin-1/2 single-tetrahedron model having $XXZ$ anisotropy and Dzyaloshinskii-Moriya interaction. This model has a two-fold degeneracy of the lowest-energy state per tetrahedron and well reproduces the magnetization curve at 0.5 K and heat capacity above 1.5 K. At lower temperatures, however, we observe a broad maximum in the heat capacity around 63 mK, demonstrating that a unique quantum ground state is selected due to extra perturbations with energy scale smaller than the instrumental resolution of INS.

cond-mat.str-el↗

arXiv2013

Coupled magnetic and ferroelectric excitations in PbFe_{1/2}Nb_{1/2}O_{3}

A neutron scattering investigation of the magnetoelectric coupling in PbFe_{1/2}Nb_{1/2}O_{3} (PFN) has been undertaken. Ferroelectric order occurs below 400 K, as evidenced by the softening with temperature and subsequent recovery of the zone center transverse optic phonon mode energy (\hbar Ω_{0}). Over the same temperature range, magnetic correlations become resolution limited on a terahertz energy scale. In contrast to the behavior of nonmagnetic disordered ferroelectrics (namely Pb(Mg,Zn)_{1/3}Nb_{2/3}O_{3}), we report the observation of a strong deviation from linearity in the temperature dependence of (\hbar Ω_{0})^{2}. This deviation is compensated by a corresponding change in the energy scale of the magnetic excitations, as probed through the first moment of the inelastic response. The coupling between the short-range ferroelectric and antiferromagnetic correlations is consistent with calculations showing that the ferroelectricity is driven by the displacement of the body centered iron site, illustrating the multiferroic nature of magnetic lead based relaxors in the dynamical regime.

cond-mat.mtrl-sci↗

arXiv2013

Development of the Magnetic Excitations of Charge-Stripe Ordered La(2-x)Sr(x)NiO(4) on Doping Towards Checkerboard Charge Order

The magnetic excitation spectrums of charge stripe ordered La(2-x)Sr(x)NiO(4) x = 0.45 and x = 0.4 were studied by inelastic neutron scattering. We found the magnetic excitation spectrum of x = 0.45 from the ordered Ni^2+ S = 1 spins to match that of checkerboard charge ordered La(1.5)Sr(0.5)NiO(4). The distinctive asymmetry in the magnetic excitations above 40 meV was observed for both doping levels, but an additional ferromagnetic mode was observed in x = 0.45 and not in the x = 0.4. We discuss the origin of crossover in the excitation spectrum between x = 0.45 and x = 0.4 with respect to discommensurations in the charge stripe structure.

cond-mat.str-el↗

arXiv2012

Two Ising-like magnetic excitations in a single-layer cuprate superconductor

There exists increasing evidence that the phase diagram of the high-transition temperature (Tc) cuprate superconductors is controlled by a quantum critical point. One distinct theoretical proposal is that, with decreasing hole-carrier concentration, a transition occurs to an ordered state with two circulating orbital currents per CuO2 square. Below the 'pseudogap' temperature T* (T* > Tc), the theory predicts a discrete order parameter and two weakly-dispersive magnetic excitations in structurally simple compounds that should be measurable by neutron scattering. Indeed, novel magnetic order and one such excitation were recently observed. Here, we demonstrate for tetragonal HgBa2CuO4+d the existence of a second excitation with local character, consistent with the theory. The excitations mix with conventional antiferromagnetic fluctuations, which points toward a unifying picture of magnetism in the cuprates that will likely require a multi-band description.

cond-mat.supr-con↗

arXiv2011

Evidence of Magnetic Correlations Among the Charge Stripe Electrons of Charge-Stripe Ordered La2NiO4.11

The magnetic excitations of charge-stripe ordered La2NiO4.11 where investigated using polarized- and unpolarized-neutron scattering to determine the magnetic excitations of the charge stripe electrons. We observed a magnetic excitation mode consistent with the gapped quasi-one-dimensional antiferromagnetic correlations of the charge stripe electrons previously observed in La(2-x)Sr(x)NiO(4) x = 1/3 and x = 0.275.

cond-mat.str-el↗

arXiv2008

Two characteristic energies in the low-energy antiferromagnetic response of the electron-doped high-temperature superconductor Nd$_{2-x}$Ce$_x$CuO$_{4+δ}$

Inelastic neutron scattering for Nd$_{2-x}$Ce$_x$CuO$_{4+δ}$ near optimal doping ($x \approx 0.155$, $T_{c} = 25 \mathrm{K}$) reveals that the dynamic magnetic susceptibility at the antiferromagnetic zone center exhibits two characteristic energies in the superconducting state: $ω_1 \approx 6.4 \mathrm{meV}$ and $ω_2 \approx 4.5 \mathrm{meV}$. These two magnetic energies agree $quantitatively$ with the $B_{1g}$ / $B_{2g}$ and $A_{1g}$ features previously observed in electronic Raman scattering, where the former is believed to indicate the maximum electronic gap and the origin of the smaller $A_{1g}$ feature has remained unexplained. The susceptibility change upon cooling into the superconducting state is inconsistent with previous claims of the existence of a magnetic resonance mode near 10 meV, but consistent with a resonance at $ω_2$.

cond-mat.supr-con↗

arXiv2008

Magnetic resonance in the model high-temperature superconductor HgBa$_2$CuO$_{4+δ}$

We present an inelastic neutron scattering study of the structurally simple single-layer compound HgBa$_2$CuO$_{4+δ}$ close to optimal doping ($T_c \approx 96$ K). A well-defined antiferromagnetic resonance with energy $ω_r = 56$ meV ($\approx 6.8 k_BT_c$) is observed below the superconducting transition temperature $T_c$. The resonance mode is energy-resolution limited and exhibits an intrinsic momentum width of about $0.2 \mathrm{\mathring{A}^{-1}}$, consistent with prior work on several other cuprates. However, the unusually large value of the mode energy implies a non-universal relationship between $ω_r$ and $T_c$ across different families of cuprates.

cond-mat.supr-con↗