arXiv subjects

D. E. McNally

Publications and source records attributed to D. E. McNally.

11 recordsLinked to original sources

arXiv2021

Charge ordering in Ir dimers in the ground state of Ba$_5$AlIr$_2$O$_{11}$

It has been well established experimentally that the interplay of electronic correlations and spin-orbit interactions in Ir$^{4+}$ and Ir$^{5+}$ oxides results in insulating J$_{\rm eff}$=1/2 and J$_{\rm eff}$=0 ground states, respectively. However, in compounds where the structural dimerization of iridum ions is favourable, the direct Ir $d$--$d$ hybridisation can be significant and takes a key role. Here, we investigate the effects of direct Ir $d$--$d$ hybridisation in comparison with electronic correlations and spin-orbit coupling in Ba$_5$AlIr$_2$O$_{11}$, a compound with Ir dimers. Using a combination of $ab$ $initio$ many-body wave function quantum chemistry calculations and resonant inelastic X-ray scattering (RIXS) experiments, we elucidate the electronic structure of Ba$_5$AlIr$_2$O$_{11}$. We find excellent agreement between the calculated and the measured spin-orbit excitations. Contrary to the expectations, the analysis of the many-body wave function shows that the two Ir (Ir$^{4+}$ and Ir$^{5+}$) ions in the Ir$_2$O$_9$ dimer unit in this compound preserve their local J$_{\rm eff}$ character close to 1/2 and 0, respectively. The local point group symmetry at each of the Ir sites assumes an important role, significantly limiting the direct $d$--$d$ hybridisation. Our results emphasize that minute details in the local crystal field (CF) environment can lead to dramatic differences in electronic states in iridates and 5$d$ oxides in general.

cond-mat.str-el↗

arXiv2019

Strain-Engineering Mott-Insulating La$_2$CuO$_4$

The transition temperature $T_\textrm{c}$ of unconventional superconductivity is often tunable. For a monolayer of FeSe, for example, the sweet spot is uniquely bound to titanium-oxide substrates. By contrast for La$_{2-\mathrm{x}}$Sr$_\mathrm{x}$CuO$_4$ thin films, such substrates are sub-optimal and the highest $T_\textrm{c}$ is instead obtained using LaSrAlO$_4$. An outstanding challenge is thus to understand the optimal conditions for superconductivity in thin films: which microscopic parameters drive the change in $T_\mathrm{c}$ and how can we tune them? Here we demonstrate, by a combination of x-ray absorption and resonant inelastic x-ray scattering spectroscopy, how the Coulomb and magnetic-exchange interaction of La$_2$CuO$_4$ thin films can be enhanced by compressive strain. Our experiments and theoretical calculations establish that the substrate producing the largest $T_\textrm{c}$ under doping also generates the largest nearest neighbour hopping integral, Coulomb and magnetic-exchange interaction. We hence suggest optimising the parent Mott state as a strategy for enhancing the superconducting transition temperature in cuprates.

cond-mat.str-el↗

arXiv2019

Resolving the nature of electronic excitations in resonant inelastic x-ray scattering

The study of elementary bosonic excitations is essential toward a complete description of quantum electronic solids. In this context, resonant inelastic X-ray scattering (RIXS) has recently risen to becoming a versatile probe of electronic excitations in strongly correlated electron systems. The nature of the radiation-matter interaction endows RIXS with the ability to resolve the charge, spin and orbital nature of individual excitations. However, this capability has been only marginally explored to date. Here, we demonstrate a systematic method for the extraction of the character of excitations as imprinted in the azimuthal dependence of the RIXS signal. Using this novel approach, we resolve the charge, spin, and orbital nature of elastic scattering, (para-)magnon/bimagnon modes, and higher energy dd excitations in magnetically-ordered and superconducting copper-oxide perovskites (Nd2CuO4 and YBa2Cu3O6.75). Our method derives from a direct application of scattering theory, enabling us to deconstruct the complex scattering tensor as a function of energy loss. In particular, we use the characteristic tensorial nature of each excitation to precisely and reliably disentangle the charge and spin contributions to the low energy RIXS spectrum. This procedure enables to separately track the evolution of spin and charge spectral distributions in cuprates with doping. Our results demonstrate a new capability that can be integrated into the RIXS toolset, and that promises to be widely applicable to materials with intertwined spin, orbital, and charge excitations.

cond-mat.str-el↗

arXiv2018

RIXS studies of magnons and bimagnons in the lightly doped cuprate La2-xSrxCuO4

We investigated the doping dependence of magnetic excitations in the lightly doped cuprate La2-xSrxCuO4 via combined studies of resonant inelastic x-ray scattering (RIXS) at the Cu L3-edge and theoretical calculations. With increasing doping, the magnon dispersion is found to be essentially unchanged, but the spectral width broadens and the spectral weight varies differently at different momenta. Near the Brillouin zone center, we directly observe bimagnon excitations which possess the same energy scale and doping dependence as previously observed by Raman spectroscopy. They disperse weakly in energy-momentum space, and are consistent with a bimagnon dispersion that is renormalized by the magnon-magnon interaction at the zone center.

cond-mat.supr-con↗

arXiv2017

Electronic and magnetic excitations in the "half-stuffed" Cu--O planes of Ba$_2$Cu$_3$O$_4$Cl$_2$ measured by resonant inelastic x-ray scattering

We use resonant inelastic x-ray scattering (RIXS) at the Cu L$_3$ edge to measure the charge and spin excitations in the "half-stuffed" Cu--O planes of the cuprate antiferromagnet Ba$_2$Cu$_3$O$_4$Cl$_2$. The RIXS line shape reveals distinct contributions to the $dd$ excitations from the two structurally inequivalent Cu sites, which have different out-of-plane coordinations. The low-energy response exhibits magnetic excitations. We find a spin-wave branch whose dispersion follows the symmetry of a CuO$_2$ sublattice, similar to the case of the "fully-stuffed" planes of tetragonal CuO (T-CuO). Its bandwidth is closer to that of a typical cuprate material, such as Sr$_2$CuO$_2$Cl$_2$, than it is to that of T-CuO. We interpret this result as arising from the absence of the effective four-spin inter-sublattice interactions that act to reduce the bandwidth in T-CuO.

cond-mat.str-el↗

arXiv2017

Damped spin excitations in a doped cuprate superconductor with orbital hybridization

A resonant inelastic x-ray scattering (RIXS) study of overdamped spin-excitations in slightly underdoped La$_{2-x}$Sr$_{x}$CuO$_4$ (LSCO) with $x=0.12$ and $0.145$ is presented. Three high-symmetry directions have been investigated: (1) the antinodal $(0,0)\rightarrow (1/2,0)$, (2) the nodal $(0,0)\rightarrow (1/4,1/4)$ and (3) the zone boundary direction $(1/2,0)\rightarrow (1/4,1/4)$ connecting these two. The overdamped excitations exhibit strong dispersions along (1) and (3), whereas a much more modest dispersion is found along (2). This is in strong contrast to the undoped compound La$_{2}$CuO$_4$ (LCO) for which the strongest dispersions are found along (1) and (2). The $t-t^{\prime}-t^{\prime\prime}-U$ Hubbard model used to explain the excitation spectrum of LCO predicts $-$ for constant $U/t$ $-$ that the dispersion along (3) scales with $(t^{\prime}/t)^2$. However, the diagonal hopping $t^{\prime}$ extracted on LSCO using single-band models is low ($t^{\prime}/t\sim-0.16$) and decreasing with doping. We therefore invoked a two-orbital ($d_{x^2-y^2}$ and $d_{z^2}$) model which implies that $t^{\prime}$ is enhanced. This effect acts to enhance the zone-boundary dispersion within the Hubbard model. We thus conclude that hybridization of $d_{x^2-y^2}$ and $d_{z^2}$ states has a significant impact on the zone-boundary dispersion in LSCO.

cond-mat.supr-con↗

arXiv2016

Doping Evolution of Magnetic Order and Magnetic Excitations in (Sr$_{1-x}$La$_x$)$_3$Ir$_2$O$_7$

We use resonant elastic and inelastic X-ray scattering at the Ir-$L_3$ edge to study the doping-dependent magnetic order, magnetic excitations and spin-orbit excitons in the electron-doped bilayer iridate (Sr$_{1-x}$La$_{x}$)$_3$Ir$_2$O$_7$ ($0 \leq x \leq 0.065$). With increasing doping $x$, the three-dimensional long range antiferromagnetic order is gradually suppressed and evolves into a three-dimensional short range order from $x = 0$ to $0.05$, followed by a transition to two-dimensional short range order between $x = 0.05$ and $0.065$. Following the evolution of the antiferromagnetic order, the magnetic excitations undergo damping, anisotropic softening and gap collapse, accompanied by weakly doping-dependent spin-orbit excitons. Therefore, we conclude that electron doping suppresses the magnetic anisotropy and interlayer couplings and drives (Sr$_{1-x}$La$_x$)$_3$Ir$_2$O$_7$ into a correlated metallic state hosting two-dimensional short range antiferromagnetic order and strong antiferromagnetic fluctuations of $J_{\text{eff}} = \frac{1}{2}$ moments, with the magnon gap strongly suppressed.

cond-mat.str-el↗

arXiv2015

From Hunds insulator to Fermi liquid: Optical spectroscopy study of K doping in BaMn$_2$As$_2$

We present optical transmission measurements that reveal a charge gap of 0.86 eV in the local moment antiferromagnetic insulator BaMn$_2$As$_2$, an order of magnitude larger than previously reported. Density functional theory plus dynamical mean field theory (DFT+DMFT) calculations correctly reproduce this charge gap only when a strong Hund's coupling is considered. Thus, BaMn$_2$As$_2$ is a member of a wider class of Mn pnictide compounds that are Mott-Hund's insulators. We also present optical reflectance for metallic 2% K doped BaMn$_2$As$_2$ that we use to extract the optical conductivity at different temperatures. The optical conductivity $σ_1$($ω$) exhibits a metallic response that is well described by a simple Drude term. Both $σ$($ω$$\rightarrow$0, T) and $ρ$(T) exhibit Fermi liquid temperature dependencies. From these measurements, we argue that a more strongly correlated Hund's metal version of the parent compounds of the iron pnictide superconductors has not yet been realized by doping this class of Hund's insulators.

cond-mat.str-el↗

arXiv2015

CaMn$_2$Sb$_2$: Spin waves on a frustrated antiferromagnetic honeycomb lattice

We present inelastic neutron scattering measurements of the antiferromagnetic insulator CaMn$_2$Sb$_2$, which consists of corrugated honeycomb layers of Mn. The dispersion of magnetic excitations has been measured along the H and L directions in reciprocal space, with a maximum excitation energy of $\approx$ 24 meV. These excitations are well described by spin waves in a Heisenberg model, including first and second neighbor exchange interactions, J$_{1}$ and J$_{2}$, in the Mn plane and also an exchange interaction between planes. The determined ratio J$_{2}$/J$_{1}$ $\approx$ 1/6 suggests that CaMn$_2$Sb$_2$ is the first example of a compound that lies very close to the mean field tricritical point, known for the classical Heisenberg model on the honeycomb lattice, where the Néel phase and two different spiral phases coexist. The magnitude of the determined exchange interactions reveal a mean field ordering temperature $\approx$ 4 times larger than the reported Néel temperature T$_{N}$ = 85 K, suggesting significant frustration arising from proximity to the tricritical point.

cond-mat.str-el↗

arXiv2014

Magnetic structure of Yb2Pt2Pb: Ising moments on the Shastry-Sutherland Lattice

Neutron diffraction measurements were carried out on single crystals and powders of Yb2Pt2Pb, where Yb moments form planes of orthogonal dimers in the frustrated Shastry-Sutherland Lattice (SSL). Yb2Pt2Pb orders antiferromagnetically at TN=2.07 K, and the magnetic structure determined from these measurements features the interleaving of two orthogonal sublattices into a 5*5*1 magnetic supercell that is based on stripes with moments perpendicular to the dimer bonds, which are along (110) and (-110). Magnetic fields applied along (110) or (-110) suppress the antiferromagnetic peaks from an individual sublattice, but leave the orthogonal sublattice unaffected, evidence for the Ising character of the Yb moments in Yb2Pt2Pb. Specific heat, magnetic susceptibility, and electrical resistivity measurements concur with neutron elastic scattering results that the longitudinal critical fluctuations are gapped with E about 0.07 meV.

cond-mat.str-el↗

arXiv2014

Antiferromagnetic Exchange, Hund's Coupling and the Origin of the Charge Gap in LaMnPO

We present inelastic neutron scattering and magnetization measurements of the antiferromagnetic insulator LaMnPO that are well described by a Heisenberg spin model. These measurements are consistent with the presence of two-dimensional magnetic correlations up to a temperature T$_{max}$ $\approx$ 700 K >> T$_{N}$ = 375 K, the Néel temperature. Optical transmission measurements show the T = 300 K direct charge gap $Δ$ = 1 eV has decreased only marginally by 500 K and suggest it decreases by only 10% at T$_{max}$. Density functional theory and dynamical mean field theory calculations reproduce a direct charge gap in paramagnetic LaMnPO only when a strong Hund's coupling J$_{H}$ = 0.9 eV is included, as well as onsite Hubbard U = 8 eV. These results show the direct charge gap in LaMnPO is rather insensitive to antiferromagnetic exchange coupling and instead is a result of the local physics governed by U and J$_{H}$.

cond-mat.str-el↗