arXiv subjects

H. M. Rønnow

Publications and source records attributed to H. M. Rønnow.

At least 37 records · Page 2Linked to original sources

arXiv2020

High-Temperature Charge-Stripe Correlations in La$_{1.675}$Eu$_{0.2}$Sr$_{0.125}$CuO$_4$

We use resonant inelastic x-ray scattering to investigate charge-stripe correlations in La$_{1.675}$Eu$_{0.2}$Sr$_{0.125}$CuO$_4$. By differentiating elastic from inelastic scattering, it is demonstrated that charge-stripe correlations precede both the structural low-temperature tetragonal phase and the transport-defined pseudogap onset. The scattering peak amplitude from charge stripes decays approximately as $T^{-2}$ towards our detection limit. The in-plane integrated intensity, however, remains roughly temperature independent. Therefore, although the incommensurability shows a remarkably large increase at high temperature, our results are interpreted via a single scattering constituent. In fact, direct comparison to other stripe-ordered compounds (La$_{1.875}$Ba$_{0.125}$CuO$_4$, La$_{1.475}$Nd$_{0.4}$Sr$_{0.125}$CuO$_4$ and La$_{1.875}$Sr$_{0.125}$CuO$_4$) suggests a roughly constant integrated scattering intensity across all these compounds. Our results therefore provide a unifying picture for the charge-stripe ordering in La-based cuprates. As charge correlations in La$_{1.675}$Eu$_{0.2}$Sr$_{0.125}$CuO$_4$ extend beyond the low-temperature tetragonal and pseudogap phase, their emergence heralds a spontaneous symmetry breaking in this compound.

cond-mat.supr-con↗

arXiv2020

Exchange Interactions Mediated by Non-Magnetic Cations in Double Perovskites

Establishing the physical mechanism governing exchange interactions is fundamental for exploring exotic phases such as the quantum spin liquids (QSLs) in real materials. In this work, we address exchange interactions in Sr2CuTe$_{1-x}$W$_{x}$O, a series of double perovskites that realize the spin-1/2 square lattice and were suggested to harbor a QSL ground state arising from random distribution of non-magnetic ions. Our {\it ab initio} multi-reference configuration interaction calculations show that replacing Te atoms with W atoms changes the dominant couplings from nearest to next-nearest neighbor explained by the crucial role of unoccupied states of non-magnetic ions in the super-superexchange mechanism. Combined with spin-wave theory simulations, our calculated exchange couplings provide an excellent description of the inelastic neutron scattering spectra of the end compounds, as well as explain the magnetic excitations in Sr2CuTe$_{0.5}$W$_{0.5}$O as emerging from the bond-disordered exchange couplings. Our results provide crucial understanding of the role of non-magnetic cations in exchange interactions paving the way to further exploration of QSL phases in bond-disordered materials.

cond-mat.str-el↗

arXiv2019

Temperature dependence of the $(π,0)$ anomaly in the excitation spectrum of the 2D quantum Heisenberg antiferromagnet

It is well established that in the low-temperature limit, the two-dimensional quantum Heisenberg antiferromagnet on a square lattice (2DQHAFSL) exhibits an anomaly in its spectrum at short-wavelengths on the zone-boundary. In the vicinity of the $(π,0)$ point the pole in the one-magnon response exhibits a downward dispersion, is heavily damped and attenuated, giving way to an isotropic continuum of excitations extending to high energies. The origin of the anomaly and the presence of the continuum are of current theoretical interest, with suggestions focused around the idea that the latter evidences the existence of spinons in a two-dimensional system. Here we present the results of neutron inelastic scattering experiments and Quantum Monte Carlo calculations on the metallo-organic compound Cu(DCOO)$_2\cdot 4$D$_2$O (CFTD), an excellent physical realisation of the 2DQHAFSL, designed to investigate how the anomaly at $(π,0)$ evolves up to finite temperatures $T/J\sim2/3$. Our data reveal that on warming the anomaly survives the loss of long-range, three-dimensional order, and is thus a robust feature of the two-dimensional system. With further increase of temperature the zone-boundary response gradually softens and broadens, washing out the $(π,0)$ anomaly. This is confirmed by a comparison of our data with the results of finite-temperature Quantum Monte Carlo simulations where the two are found to be in good accord. At lower energies, in the vicinity of the antiferromagnetic zone centre, there was no significant softening of the magnetic excitations over the range of temperatures investigated.

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↗

arXiv2018

Exact diagonalization study of the Hubbard-parametrized four-spin ring exchange model on a square lattice

We have used exact numerical diagonalization to study the excitation spectrum and the dynamic spin correlations in the $s=1/2$ next-next-nearest neighbor Heisenberg antiferromagnet on the square lattice, with additional 4-spin ring exchange from higher order terms in the Hubbard expansion. We have varied the ratio between Hubbard model parameters, $t/U$, to obtain different relative strengths of the exchange parameters, while keeping electrons localized. The Hubbard model parameters have been parametrized via an effective ring exchange coupling, $J_r$, which have been varied between 0$J$ and 1.5$J$. We find that ring exchange induces a quantum phase transition from the $(π, π)$ ordered Neèl state to a $(π/2, π/2)$ ordered state. This quantum critical point is reduced by quantum fluctuations from its mean field value of $J_r/J = 2$ to a value of $\sim 1.1$. At the quantum critical point, the dynamical correlation function shows a pseudo-continuum at $q$-values between the two competing ordering vectors.

cond-mat.str-el↗

arXiv2018

Controlling the helicity of magnetic skyrmions in a $β$-Mn-type high-temperature chiral magnet

Magnetic helices and skyrmions in noncentrosymmetric magnets are representative examples of chiral spin textures in solids. Their spin swirling direction, often termed as the magnetic helicity and defined as either left-handed or right-handed, is uniquely determined by the Dzyaloshinskii-Moriya interaction (DMI) in fixed chirality host crystals. Thus far, there have been relatively few investigations of the DMI in metallic magnets as compared with insulating counterparts. Here, we focus on the metallic magnets Co$_{8-x}$Fe$_x$Zn$_8$Mn$_4$ (0 $\leq$ $x$ $\leq$ 4.5) with a $β$-Mn-type chiral structure and find that as $x$ varies under a fixed crystal chirality, a reversal of magnetic helicity occurs at $x_\mathrm{c}$ $\sim$ 2.7. This experimental result is supported by a theory based on first-principles electronic structure calculations, demonstrating the DMI to depend critically on the electron band filling. Thus by composition tuning our work shows the sign change of the DMI with respect to a fixed crystal chirality to be a universal feature of metallic chiral magnets.

cond-mat.str-el↗

arXiv2018

Disordered skyrmion phase stabilized by magnetic frustration in a chiral magnet

Magnetic skyrmions are vortex-like topological spin textures often observed to form a triangular-lattice skyrmion crystal in structurally chiral magnets with Dzyaloshinskii-Moriya interaction. Recently $β$-Mn structure-type Co-Zn-Mn alloys were identified as a new class of chiral magnet to host such skyrmion crystal phases, while $β$-Mn itself is known as hosting an elemental geometrically frustrated spin liquid. Here we report the intermediate composition system Co$_7$Zn$_7$Mn$_6$ to be a unique host of two disconnected, thermal-equilibrium topological skyrmion phases; one is a conventional skyrmion crystal phase stabilized by thermal fluctuations and restricted to exist just below the magnetic transition temperature $T_\mathrm{c}$, and the other is a novel three-dimensionally disordered skyrmion phase that is stable well below $T_\mathrm{c}$. The stability of this new disordered skyrmion phase is due to a cooperative interplay between the chiral magnetism with Dzyaloshinskii-Moriya interaction and the frustrated magnetism inherent to $β$-Mn.

cond-mat.str-el↗

arXiv2018

Negative-pressure-induced helimagnetism in ferromagnetic cubic perovskites Sr$_{1-x}$Ba$_{x}$CoO$_{3}$

Helimagnetic materials are identified as promising for novel spintronic applications. Since helical spin order is manifested as a compromise of competing magnetic exchange interactions, its emergence is limited by unique constraints imposed by the crystalline lattice and the interaction geometries, as exemplified by the multiferroic perovskite manganites with large orthorhombic distortion. Here we show that a simple cubic perovskite SrCoO$_3$ with room-temperature ferromagnetism has the potential to host helimagnetic order upon isotropic lattice expansion. Increasing the Ba content $x$ in Sr$_{1-x}$Ba$_x$CoO$_3$ continuously expands the cubic lattice, eventually suppressing the ferromagnetic order near $x$=0.4, where helimagnetic correlations are observed as incommensurate diffuse magnetic scattering by neutron diffraction measurements. The emergence of helimagnetism is semi-quantitatively reproduced by first-principles calculations, leading to the conjecture that a simple cubic lattice with strong $d$-$p$ hybridisation can exhibit a variety of novel magnetic phases originating from competing exchange interactions.

cond-mat.str-el↗

arXiv2018

Electric field-driven topological phase switching and skyrmion lattice metastability in magnetoelectric Cu$_{2}$OSeO$_{3}$

Due to their topological protection and nanometric size, magnetic skyrmions are anticipated to form components of new high-density memory technologies. In metallic systems skyrmion manipulation is achieved easily under a low density electric current flow, although the inevitable thermal dissipation ultimately limits the energy efficacy of potential applications. On the other hand, a near dissipation-free skyrmion and skyrmion phase manipulation is expected by using electric \emph{fields}, thus meeting better the demands of an energy-conscious society. In this work on an insulating chiral magnet Cu$_{2}$OSeO$_{3}$ with magnetoelectric coupling, we use neutron scattering to demonstrate directly i) the creation of metastable skyrmion states over an extended range in magnetic field and temperature, and ii) the in-situ electric field-driven switching between topologically distinct phases; the skyrmion phase and a competing non-topological cone phase. For our accessible electric field range, the phase switching is achieved in a high temperature regime, and the remnant (E=0) metastable skyrmion state is thermally volatile with an exponential lifetime on hour timescales. Nevertheless, by taking advantage of the demonstrably longer-lived metastable skyrmion states at lower temperatures, a truly non-volatile and near dissipation-free topological phase change memory function is promised in magnetoelectric chiral magnets.

cond-mat.str-el↗

arXiv2018

$A$-cation control of magnetoelectric quadrupole order in $A$(TiO)Cu$_4$(PO$_4$)$_4$ ($A$ = Ba, Sr, and Pb)

Ferroic magnetic quadrupole order exhibiting macroscopic magnetoelectric activity is discovered in the novel compound $A$(TiO)Cu$_4$(PO$_4$)$_4$ with $A$ = Pb, which is in contrast with antiferroic quadrupole order observed in the isostructural compounds with $A$ = Ba and Sr. Unlike the famous lone-pair stereochemical activity which often triggers ferroelectricity as in PbTiO$_3$, the Pb$^{2+}$ cation in Pb(TiO)Cu$_4$(PO$_4$)$_4$ is stereochemically inactive but dramatically alters specific magnetic interactions and consequently switches the quadrupole order from antiferroic to ferroic. Our first-principles calculations uncover a positive correlation between the degree of $A$-O bond covalency and a stability of the ferroic quadrupole order.

cond-mat.mtrl-sci↗

arXiv2018

Direct observation of multi-spinon excitations outside of the two-spinon continuum in the antiferromagnetic spin chain cuprate Sr2CuO3

One-dimensional (1D) magnetic insulators have attracted significant interest as a platform for studying emergent phenomena such as quasiparticle fractionalization and quantum criticality. The antiferromagnetic Heisenberg chain of spins-1/2 is an important reference system; its elementary excitations are spin-1/2 quasiparticles called spinons that are always created in pairs. However, while inelastic neutron scattering (INS) experiments routinely observe the excitation continuum associated with two-spinon states, the presence of more complex dynamics associated with four-spinon states has only been inferred from comparison with theory. Here, we show that resonant inelastic x-ray scattering (RIXS) is capable of accessing the four-spinon excitations directly, in a spectroscopic region separated from the two-spinon continuum. Our results provide the first direct measurement of four-spinon excitations, which is made possible by the fundamentally different correlation functions probed by RIXS compared to INS. This advance holds great promise as a tool in the search for novel quantum states, in particular quantum spin liquids.

cond-mat.str-el↗

arXiv2018

Spin-Orbital Excitations in Ca$_{2}$RuO$_4$ Revealed by Resonant Inelastic X-ray Scattering

The strongly correlated insulator Ca$_{2}$RuO$_4$ is considered as a paradigmatic realization of both spin-orbital physics and a band-Mott insulating phase, characterized by orbitally selective coexistence of a band and a Mott gap. We present a high-resolution oxygen $K$-edge resonant inelastic X-ray scattering study of the antiferromagnetic Mott insulating state of Ca$_{2}$RuO$_4$. A set of low-energy ($\sim$80 and 400 meV) and high-energy ($\sim$1.3 and 2.2 eV) excitations are reported that show strong incident light polarization dependence. Our results strongly support a spin-orbit coupled band-Mott scenario and explore in detail the nature of its exotic excitations. Guided by theoretical modelling, we interpret the low-energy excitations as a result of composite spin-orbital excitations. Their nature unveil the intricate interplay of crystal-field splitting and spin-orbit coupling in the band-Mott scenario. The high-energy excitations correspond to intra-atomic singlet-triplet transitions at an energy scale set by the Hund's coupling. Our findings give a unifying picture of the spin and orbital excitations in the band-Mott insulator Ca$_{2}$RuO$_4$.

cond-mat.str-el↗

arXiv2017

Charge-Stripe Order and Superconductivity in $\mathrm{Ir_{1-x}Pt_xTe_2}$

A combined resistivity and hard x-ray diffraction study of superconductivity and charge ordering in $\mathrm{Ir_{1-x}Pt_xTe_2}$, as a function of Pt substitution and externally applied hydrostatic pressure, is presented. Experiments are focused on samples near the critical composition $x_c\sim 0.045$ where competition and switching between charge order and superconductivity is established. We show that charge order as a function of pressure in $\mathrm{Ir_{0.95}Pt_{0.05}Te_{2}}$ is preempted - and hence triggered - by a structural transition. Charge ordering appears uniaxially along the short crystallographic (1,0,1) domain axis with a $\mathrm{(\frac{1}{5},0,\frac{1}{5})}$ modulation. Based on these results we draw a charge-order phase diagram and discuss the relation between stripe ordering and superconductivity.

cond-mat.supr-con↗

arXiv2017

Magnetic structure of Ba(TiO)Cu$_4$(PO$_4$)$_4$ probed using spherical neutron polarimetry

The antiferromagnetic compound Ba(TiO)Cu$_4$(PO$_4$)$_4$ contains square cupola of corner-sharing CuO$_4$ plaquettes, which were proposed to form effective quadrupolar order. To identify the magnetic structure, we have performed spherical neutron polarimetry measurements. Based on symmetry analysis and careful measurements we conclude that the orientation of the Cu$^{2+}$ spins form a non-collinear in-out structure with spins approximately perpendicular to the CuO$_4$ motif. Strong Dzyaloshinskii-Moriya interaction naturally lends itself to explain this phenomenon. The identification of the ground state magnetic structure should serve well for future theoretical and experimental studies into this and closely related compounds.

cond-mat.str-el↗

arXiv2017

Skyrmion formation in a bulk chiral magnet at zero magnetic field and above room temperature

We report that in a $β$-Mn-type chiral magnet Co$_9$Zn$_9$Mn$_2$, skyrmions are realized as a metastable state over a wide temperature range, including room temperature, via field-cooling through the thermodynamic equilibrium skyrmion phase that exists below a transition temperature $T_\mathrm{c}$ $\sim$ 400 K. The once-created metastable skyrmions survive at zero magnetic field both at and above room temperature. Such robust skyrmions in a wide temperature and magnetic field region demonstrate the key role of topology, and provide a significant step toward technological applications of skyrmions in bulk chiral magnets.

cond-mat.str-el↗

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

Magnetic excitations from the two-dimensional interpenetrating Cu framework in Ba$_2$Cu$_3$O$_4$Cl$_2$

We report detailed neutron scattering studies on Ba$_2$Cu$_3$O$_4$Cl$_2$. The compound consists of two interpenetrating sublattices of Cu, labeled as Cu$_{\rm A}$ and Cu$_{\rm B}$, each of which forms a square-lattice Heisenberg antiferromagnet. The two sublattices order at different temperatures and effective exchange couplings within the sublattices differ by an order of magnitude. This yields an inelastic neutron spectrum of the Cu$_{\rm A}$ sublattice extending up to 300 meV and a much weaker dispersion of Cu$_{\rm B}$ going up to around 20 meV. Using a single-band Hubbard model we derive an effective spin Hamiltonian. From this, we find that linear spin-wave theory gives a good description to the magnetic spectrum. In addition, a magnetic field of 10 T is found to produce effects on the Cu$_{\rm B}$ dispersion that cannot be explained by conventional spin-wave theory.

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↗